Real Madrid came back from a goal down to beat Villarreal 2-1 on the final day of the La Liga season but it wasn't enough as Atletico Madrid took the title.
Teenager Yeremi Pino scored early in the first half for Villarreal before Karim Benzema and Luka Modric scored late in the second.
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In the end, the result didn't matter as Atletico -- who had a two point cushion over Madrid heading into the game -- beat Real Valladolid 2-1.
"We had to win and then see what happened with Atletico in Valladolid. They won and did what they had to do, we have to congratulate them," Casemiro said after the game.
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"You're aware of what is happening but the most important thing is to focus on yourself. We were losing, we fought, we worked, we gave everything, as this crest demands. We did what we had to do, win the game. Congratulations to Atletico Madrid.
"It is complicated, after more than 60 injuries, COVID-19, there are no excuses but it is a bit of everything. We were one game from winning La Liga. We are all proud, it was a difficult year for us with so many injuries. A lot of fighting, a lot of work, a really difficult year for us."
Pino put Villarreal ahead after just 20 minutes when he received a short pass from Gerard Moreno which he hit past Thibaut Courtois.
Luka Modric had a chance to pull the sides level on 34 minutes when he got a foot to a rebounded shot but sent it wide.
Madrid thought they'd found their equaliser again on 55 minutes when Benzema put the ball in the back of the net. However, VAR replays showed he was offside and the goal was disallowed.
The France international found the net again from the edge of the box on 87 minutes before Modric followed up with a second goal two minutes into added time.
Alex Kirkland contributed information to this report.