The Spanish champions, who defeated Real Madrid 2-1 in the league at the weekend, found themselves 2-0 behind by the 30th minute at the Georgios Karaiskaki, courtesy of goals from Arthur Masuaku and Ibrahim Afellay.
Mario Mandzukic reduced the arrears for the visitors in the first-half, but Olympiacos reclaimed their two-goal lead in the 73rd minute when Konstantinos Mitroglou found the back of net.
Antoine Griezmann’s late strike gave Atletico Madrid some hope, but it was too little too late as last season’s finalists started their 2014/15 European campaign with a loss.
And Simeone, who praised Olympiacos’ clinical nature in front of goal, urged his side to return to winning ways in their next Champions League outing.
“We posed a threat throughout, but Olympiacos were very tough indeed”, the manager told UEFA’s official site.
“What made the difference was that they were more clinical with the chances that came their way.
“There is no doubt this was a very negative result for us and Olympiacos are now in a very good position. We feel we have a responsibility to bounce back.”
Atletico Madrid will next play Juventus, who currently top Group A after their 2-0 win over Malmo in the group’s other match last night, in early October.
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