Sunday's victory, which came courtesy of two strikes from Diego Costa before Nolito's consolation for the visitors, sees Atleti draw level with Barcelona at the top of La Liga with eight wins from eight games.
And such was the dominance of their display, Simeone hailed the performance as arguably the best he has witnessed during his time at the helm.
He said: It's possibly the best since I've been in charge. There were no cracks or potholes in the group. We had total control, with numerous scoring chances and a lot of pressure in their half. We delivered a near perfect first half.
Costa's two goals - his seventh and eighth of the campaign - led Simeone to hail his striker's sensational display and the Brazilian admitted he was content with the performance of the team but disappointed to miss a first half penalty.
I hate to miss penalties, but I'll take another, he said. In the first half we had many chances - our intensity wasn't quite the same but we got the win against a good team.
The Brazilian's international future has been debated at length this week, with the 24-year-old keen to represent Spain rather than the country of his birth, but he insists the topic is not affecting his performances on the pitch.
