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While Cristiano Ronaldo is maintaining his record-setting Champions League level, Barcelona have become barely recognisable as a European power.
Ronaldo struck deep into stoppage time as Manchester United snatched a 2-1 come-from-behind win over Villarreal, his record-extending 136th goal coming in his 178th game - one more than any other player.
That goal moved United off the bottom of Group F, but five-time European champions Barcelona remained last in Group E with another 3-0 loss.
Barca finished with 10 men in a humbling defeat at Benfica, two weeks after being swatted aside at home by Bayern Munich.
Bayern eased clear atop the group by routing Dynamo Kyiv 5-0 with Robert Lewandowski scoring twice in the first half for the 2020 champions.
Title-holders Chelsea lost 1-0 at Juventus after being caught cold with a goal within seconds of the restart for the second half.
Atalanta won 1-0 at home in Italy against Young Boys to lead their group, one point ahead of United before they meet next at Old Trafford on October 20.
United were having another tough evening as Villarreal led in the 53rd minute from Paco Alcacer's goal in a rematch of the Europa League final in May won by the Spanish club.
The hosts got a spectacular leveller in the 60th when defender Alex Telles netted a volley from a Bruno Fernandes pass.
It was a goal after five minutes of stoppage time that sent United to a 2-1 loss at Young Boys two weeks ago, but this time the goal went their way.
Ronaldo got the ball back from substitute Jesse Lingard in the penalty area and fired it in before running off to celebrate shirtless with a frenetic crowd that included longtime fan Usain Bolt.
"It's just what he has done throughout his career," United manager Ole Gunnar Solskjaer said.
"He is so strong mentally. He stays in the game... And when he gets that one chance, it's a goal."
It was Ronaldo's fifth goal in five games back at the club he left after losing the 2009 final to Barcelona.
Barca have lost the aura they had before Lionel Messi's departure for Paris Saint-Germain.
"There's no point in comparing this with Barcelona teams of years gone by," said coach Ronald Koeman, a brace from Darwin Nunez and Rafa Silva goal condemning his side to defeat.
Italy's run to the European Championship title in the summer was fuelled by goals from Federico Chiesa of Juventus and Matteo Pessina of Atalanta.
Both were on target on Wednesday to give their respective sides the points.
Zenit St Petersburg beat 10-man Malmo 4-0 in one of the early kick-offs.
In Group H, Salzburg's Karim Adeyemi netted two penalties in a 2-1 home win over Lille while Sevilla drew 1-1 at Wolfsburg, relying on a penalty converted by Croatian veteran Ivan Rakitic in the 86th.