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Brennan Johnson's well-taken opener marked his sixth goal in as many games across all competitions before James Maddison's first-half finish had Spurs leading 2-0 at the break.
It was just the second time that Tottenham lost a Premier League game it led by two goals in its past 166 matches, and Postecoglou fumed at the full-time whistle.
The Tottenham manager said: "Disappointing, frustrated and absolutely gutted with that. It's the worst defeat since I've been here.
"Unacceptable second half, and nowhere near where we should be. We got carried away with how we were going.
"We kind of accepted our fate [in the second half] and it is hard to understand as we've not done that while I've been here. We paid the price.
"The problem is we are travelling along too smoothly, football and life will trip you up if you get too far ahead of yourself."
The result also marked the 10th time that Tottenham has lost a Premier League game in which it led by two or more goals, becoming the first club to hit double figures for this unwanted record.
"There is no message," the Australian said when asked what he would tell his players. "It is a terrible loss for us, as bad as it gets. There is only one way to fix it and that's my responsibility.
"We lost all our duels and if you're not competitive it is not going to work; we were not competitive.
"They all go on international duty the majority of them, they will process it individually and I will process it when everyone gets back."
This week, Manchester United hosts Tottenham Hotspur in the Premier League's marquee match, featuring two underperforming teams vying for European qualification. Both clubs aim to turn their fortunes around after falling short last season, but five games into the new campaign, neither has established itself as a top contender for a Champions League spot.
Currently, Manchester United sits at 11th place while Tottenham is just above them at 10th, with both teams accumulating only seven points ahead of their clash at Old Trafford on Sunday. United's situation worsened after a disappointing draw against Twente in the Europa League, while Spurs managed to relieve some pressure with a victory over Qarabag.
Both managers, Erik ten Hag and Ange Postecoglou, are feeling the heat early in the season. A loss in this match could intensify criticism of either coach, raising the stakes for this encounter.
Historically, Manchester United has been dominant at home against Tottenham, winning 24 Premier League matches—only Arsenal has more home wins against a single opponent. Given this history, it's no surprise that statistical projections favor United, albeit narrowly. In simulations conducted by the Opta supercomputer, United has a 41.1% chance of winning, Spurs have a 34.6% chance, and the remaining 24.3% is projected for a draw.
Tottenham, however, comes into this match with a positive streak, remaining unbeaten in their last three Premier League games against United, with one win and two draws following a stretch of four consecutive losses.
United's season has been marked by an inability to capitalize on scoring opportunities. In their most recent match against Crystal Palace, they dominated possession but failed to convert their five clear chances into goals, resulting in a frustrating goalless draw. With injuries affecting key players like Rasmus Hojlund and Bruno Fernandes yet to find the net this season, United's offensive struggles have been evident.
The team has recorded an expected goals (xG) tally of 9.6, the third highest in the league, but has only managed to score five times, indicating a significant shortfall. New signing Joshua Zirkzee has been highlighted for his xG, and Marcus Rashford, who may return to the starting lineup, has a solid history against Spurs.
Tottenham's form has been inconsistent, though they rebounded from two Premier League losses with a crucial win against Brentford. The team has shown resilience, gaining points from losing positions, but their away form has been a concern. Under Postecoglou, Spurs have struggled on the road, garnering only 14 points from their last 15 away matches.
If they are to contend for a top-four finish, improving away performance is critical, starting with this fixture against a direct rival.
For Manchester United, Bruno Fernandes is pivotal, having taken the most shots without scoring in the league this season. His involvement in attacking sequences has been significant, making him a crucial figure for the Red Devils.
For Tottenham, Son Heung-min is expected to play a key role, having created the most chances from open play in the Premier League. His ability to contribute both goals and assists will be vital for Spurs as they seek to capitalize on their scoring opportunities against United.
As both teams look to find their footing in the league, this clash at Old Trafford promises to be an exciting encounter filled with pressure and potential turning points for both clubs.
Spurs were held 1-1 by Leicester City in their opening match but showed no such signs of profligacy against Everton, with Bissouma setting the tone inside 14 minutes with a 20-yard rocket, his first goal for the club.
Jordan Pickford's howler 11 minutes later after dallying too long on the ball gifted Son a simple finish at Tottenham Hotspur Stadium as Everton, beaten 3-0 by Brighton in its opening match last week, caved under the pressure.
Everton offered a little more attacking impetus in the second period with the arrival of recent signings Dame Ndiaye and Jesper Lindstrom, the latter forcing Guglielmo Vicario into a rare save.
However, Cristian Romero's towering header on his 100th Tottenham appearance put the hosts out of reach on 71 minutes, followed soon after by Son's second after a brilliant run from Micky van de Ven.
Everton remains planted to the bottom of the early standings as one of four sides with zero points after two matches, while Tottenham has four points from its two games.
Everton has now lost their its two games by an aggregate 7-0 scoreline, with this marking the first occasion it has lost its first two games in a top-flight season by three-plus goals in its history.
It is a familiar losing feeling for the Toffees, as it becomes just the second side to taste defeat in its opening two Premier League games in three successive campaigns after Bournemouth between 2015-2016 and 2017-2018.
But it was happy days for Postecoglou, the Australian seeing the attacking prowess of his side on full display.
But he said Bissouma "still has work to do" to win back his full trust, although marking his Tottenham return with a goal will certainly help.
Bissouma was suspended by Spurs after filming himself inhaling nitrous oxide and missed the 1-1 draw with Leicester City as a result.
Asked about Bissouma after the win, Postecoglou said: "It's a good start. He's still got work to do.
"I'm not doubting his footballing quality. We want to make him the best version of himself. That starts off the field as much as on it."
After beating Everton by four-or-more goals for the fourth time in the Premier League, Postecoglou insisted there is still more to come from his side.
"The performance was good. It's really encouraging for us," he said. "There is more [to come]. We want to keep performing."
Asked if he will add to his squad before next week's transfer deadline, Postecoglou added: "I think we have spent wisely.
Ange Postecoglou has confirmed Yves Bissouma has been suspended for Tottenham's opening game of the Premier League campaign against Leicester.
Bissouma, who made 28 appearances last season, posted a video of himself inhaling nitrous oxide on social media last weekend.
The incident occurred hours after Spurs' final pre-season clash, where they lost 3-2 to Bayern Munich in the Visit Malta Cup.
The 27-year-old later issued an apology, saying: "I want to apologise for these videos. This was a severe lack of judgement.
"I understand how serious this is and the health risks involved, and I also take my responsibility as a footballer and role model very seriously.”
However, Spurs have since taken the decision to exclude the midfielder from the squad for their trip to the King Power Stadium on Monday.
"I've been in the game for a long time. When a situation like this arises, I've tried to look at them in a couple of ways," Postecoglou said in his pre-match press conference.
"First, there's a person. That's Biss and he's made a poor decision.
"There are still sanctions involved, and some of those are educational. The second part of that is he's a footballer, with responsibilities.
"He won't be available on Monday. We've suspended him for Monday's game. He needs to build that trust back with both me and the group.
"The door is open for him and hopefully we can help him realise the decisions he makes impact the group.
"[It's down to] behaviour, it's that simple. It's about making better decisions. He was very apologetic to me, the club and everyone involved, but that's just part of it."
Ange Postecoglou has confirmed Yves Bissouma has been suspended for Tottenham's opening game of the Premier League campaign against Leicester.
Bissouma, who made 28 appearances last season, posted a video of himself inhaling nitrous oxide on social media last weekend.
The incident occurred hours after Spurs' final pre-season clash, where they lost 3-2 to Bayern Munich in the Visit Malta Cup.
The 27-year-old later issued an apology, saying: "I want to apologise for these videos. This was a severe lack of judgement.
"I understand how serious this is and the health risks involved, and I also take my responsibility as a footballer and role model very seriously.”
However, Spurs have since taken the decision to exclude the midfielder from the squad for their trip to the King Power Stadium on Monday.
"I've been in the game for a long time. When a situation like this arises, I've tried to look at them in a couple of ways," Postecoglou said in his pre-match press conference.
"First, there's a person. That's Biss and he's made a poor decision.
"There are still sanctions involved, and some of those are educational. The second part of that is he's a footballer, with responsibilities.
"He won't be available on Monday. We've suspended him for Monday's game. He needs to build that trust back with both me and the group.
"The door is open for him and hopefully we can help him realise the decisions he makes impact the group.
"[It's down to] behaviour, it's that simple. It's about making better decisions. He was very apologetic to me, the club and everyone involved, but that's just part of it."
Ange Postecoglou has confirmed Yves Bissouma has been suspended for Tottenham's opening game of the Premier League campaign against Leicester.
Bissouma, who made 28 appearances last season, posted a video of himself inhaling nitrous oxide on social media last weekend.
The incident occurred hours after Spurs' final pre-season clash, where they lost 3-2 to Bayern Munich in the Visit Malta Cup.
The 27-year-old later issued an apology, saying: "I want to apologise for these videos. This was a severe lack of judgement.
"I understand how serious this is and the health risks involved, and I also take my responsibility as a footballer and role model very seriously.”
However, Spurs have since taken the decision to exclude the midfielder from the squad for their trip to the King Power Stadium on Monday.
"I've been in the game for a long time. When a situation like this arises, I've tried to look at them in a couple of ways," Postecoglou said in his pre-match press conference.
"First, there's a person. That's Biss and he's made a poor decision.
"There are still sanctions involved, and some of those are educational. The second part of that is he's a footballer, with responsibilities.
"He won't be available on Monday. We've suspended him for Monday's game. He needs to build that trust back with both me and the group.
"The door is open for him and hopefully we can help him realise the decisions he makes impact the group.
"[It's down to] behaviour, it's that simple. It's about making better decisions. He was very apologetic to me, the club and everyone involved, but that's just part of it."
Son Heung-min scored late on as Tottenham came from behind to beat Luton 2-1.
Spurs produced another second-half rally to claim a crucial win in the race for Champions League qualification.
Bayern Munich striker Harry Kane will make a return to the Tottenham Hotspur Stadium to face his former club in August.