The 26-year-old striker, who had last scored in November 2013 in a World Cup playoff for Greece, grabbed the third goal in what was a stunning victory for the Greek champions in their Group A opener.
Mitroglou was at Fulham last season but struggled with injury and loss of form and made only one start for the London club as they were relegated from the Premier League.
“I came to Olympiakos to help them and for the club also to help me," Mitroglou told reporters.
"I know what I can do and today I just played the way I know how to play football. It is important that (Olympiakos coach) Michel is in the dugout. He knows me and we have mutual trust and after finding my feet again tonight I feel absolutely fine."
Olympiakos were handed a dream start when slack Atletico marking at a corner allowed young French defender Arthur Masuaku to drill home a low shot.
It got even better for the hosts just after the half-hour mark when Ibrahim Afellay doubled the advantage.
Mario Mandzukic pulled a goal back for Atletico - last year’s Champions League runners-up - seven minutes before halftime, but the visitors fell behind again to Mitroglou’s 73rd-minute strike on the turn from Pajtim Kasami’s centre.
Atletico substitute Antoine Griezmann set up a tense finish with a close-range strike with four minutes left, but Michel's team clung on for victory.
It was a win which left Atletico coach Diego Simeone, who was serving a touchline ban, with plenty to mull over.
"Obviously this was a very negative result for us," said the Argentine.
"Clearly Olympiakos are in a good position and what we feel now is a higher sense of responsibility to turn things around.
“We did threaten all throughout the match, but they (Olympiakos) were very determined and they got a valuable win."
NO FEAR
Masuaku, who scored the opener on his Champions League debut, believes Olympiakos have no need to fear the bigger clubs.
“We are a young team, but we showed today that we have good chemistry,” the 20-year-old said.
“This helps in football, when you have a strong connection with your team mates then you play good football and score goals. I don’t think we should fear anyone based on the way we have played," the former Valenciennes player added.
Atletico's French forward Antoine Griezmann praised the home fans, who created an intimidating atmosphere that helped contribute to a memorable night for the hosts.
“I take my hat off to the Olympiakos fans; they were incredible and made a difference,” he told reporters.
“We didn’t underestimate Olympiakos, our coach had told us that we would be up against an excellent team and it showed on the pitch. We have to try not to repeat the same mistakes in the next match if we want to bounce back.”
(Editing by Justin Palmer and Toby Davis)
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