Arsenal ended Liverpool's bid to set a new Premier League points record with a 2-1 win over the champions, while Manchester City pushed Bournemouth closer to relegation with a 2-1 victory on Wednesday.
Jurgen Klopp's side needed to win their final three games of the season to break Manchester City's record of 100 points set in 2018.
They were on course when Sadio Mane opened the scoring with a clinical finish from Andrew Robertson's cross at the Emirates Stadium.
But two careless mistakes condemned Liverpool to a third league defeat this season.
Virgil van Dijk's wayward backpass went straight to Alexandre Lacazette, who rounded Reds keeper Alisson Becker to slot home in the 32nd minute.
1 - Arsenal's equaliser came following Virgil van Dijk's first error leading to a goal in the Premier League since March 2019 (v Fulham), while it was also the Gunners' first shot of the game. Gift. pic.twitter.com/N6IlV0hgJL— OptaJoe (@OptaJoe) July 15, 2020
Alisson was guilty of an equally costly blunder when his pass out was intercepted by Lacazette and he picked out 20-year-old Reiss Nelson for a cool close-range finish.
Liverpool have failed to win three of their five matches since clinching the title.
They have 93 points and with just two games left and can only reach 99 at the end of their first title-winning campaign for 30 years.
"Twice there was a massive lack of concentration. We took a break after 1-0. Those two moments killed the game for us," Klopp said.
"You can't win games when you concede chances like that. We have to learn from it, 100 per cent."
Arsenal climb to ninth place as they chase qualification for the Europa League.
1+1 - Alexandre Lacazette is the first @Arsenal player to score and assist against the side starting the day top of the league since Thierry Henry vs Man Utd in January 2007. Statement. pic.twitter.com/ioCNSEjSeD— OptaJoe (@OptaJoe) July 15, 2020
Mikel Arteta's side go into Saturday's FA Cup semi-final against Manchester City in good spirits after bouncing back from Sunday's defeat at north London rivals Tottenham.
"In terms of energy and happiness in the dressing room before the semi-final, it's a good medicine," Arteta said.
"To beat this team you have to have moments in the game when you take your chances, defend and have a bit of luck."
Manchester City had enjoyed a big win off the field already this week with their appeal to the Court of Arbitration for Sport overturning a two-season ban from playing in European competitions, freeing up Pep Guardiola's men to play in the Champions League next season.
111 - Pep Guardiola has won 111 of his first 150 Premier League games, six more than any other coach at this stage of their career in the competition. Master. pic.twitter.com/TJ3OWsZf8X— OptaJoe (@OptaJoe) July 15, 2020
Guardiola left Aymeric Laporte, Kevin De Bruyne, Raheem Sterling and Riyad Mahrez on the bench against Bournemouth to keep them fresh for Wembley, but City still had too much quality in the form of David Silva and Gabriel Jesus.
Silva showed why he will be so missed when he leaves at the end of the season, the midfielder curling a free-kick in off the underside of the crossbar after six minutes.
Jesus was ruthless in the 39th minute as he wriggled between two weak Bournemouth challenges before firing into the far corner to score for the third consecutive game.
5 - The 16 instances of a Spaniard reaching 10 Premier League assists in a single season are made up of only five players:— OptaJoe (@OptaJoe) July 15, 2020
x6 | Cesc Fábregas
x4 | David Silva
x2 | Santi Cazorla
x2 | Juan Mata
x2 | José Antonio Reyes
City finally conceded for the first time in five home games since the restart when David Brooks turned home Callum Wilson's cross two minutes from time.
"It was a really difficult game. We started well in the first 10 or 15 minutes of the second half but then we had a problem in our build-up," Guardiola said.
Defeat leaves Bournemouth still three points adrift of safety from Watford and West Ham, who face each other on Friday.
Wolves held, but Tottenham won
Wolves remain three points adrift of the Champions League places with just two games to play after Chris Wood's 96th-minute spot-kick gave Burnley a 1-1 draw at Turf Moor.
It was not until 14 minutes from time that the visitors broke the deadlock thanks to Raul Jimenez's stunning strike on the half-volley.
In stoppage-time, Mike Dean pointed to the spot for a handball by Matt Doherty despite the Irishman seemingly being impeded by Wood's attempt at an overhead kick.
200 – Harry Kane’s strike is his 200th club career goal in his 350th appearance in all competitions, with 184 of these coming for Spurs (Millwall (9), Leyton Orient (5) & Leicester (2)). Beacon. pic.twitter.com/0hcENvkQz7— OptaJoe (@OptaJoe) July 15, 2020
Tottenham won 3-1 at Newcastle to keep their chances of European football next season on track by moving up to seventh.
Son Heung-min's shot crept in at Martin Dubravka's near post to open the scoring for Tottenham
Matt Ritchie got Newcastle's equaliser, but Harry Kane restored Tottenham's lead and the England captain added his second in the final minute.
Feature image courtesy: AFP / Paul Childs