Emery got the better of Simeone in a tight game at the Metropolitano
Villarreal made it two wins from two this season as they stunned Atletico Madrid by winning 2-0 at the Metropolitano on Sunday.
A hard-fought encounter looked likely to end goalless until Yeremy Pino opened the scoring in the 73rd minute, taking advantage of a stray Nahuel Molina pass.
Molina's evening went from bad to worse when he was sent off in stoppage time and with 10-man Atletico pushing for an equaliser, Gerard Moreno sealed the three points on the break.
Unai Emery's side now have six points from six, while Diego Simeone's team have been stopped in their tracks after an impressive win at Getafe in the first week of the season.
Villarreal travel to Getafe next weekend and Atletico are at Valencia.
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