League leaders Atletico sit three points clear of both Barcelona and Real Madrid after 22 matches following last weekend, when they beat Real Sociedad while both their rivals dropped points.
They have lost just once in La Liga all season, and have an excellent pairing up front in Diego Costa and David Villa.
But ahead of the first leg of Atletico's Copa del Rey semi-final first leg at neighbours Real on Wednesday, Simeone said he does not believe his side can be crowned champions of Spain.
"I insist - I don't think we can win the league," he said.
"Our motto is silence and work and they will not make me believe something I don't.
"If we look at the last decade at best we've finished third, 15, 20 or 30 points behind, so I don't think we can."
Simeone's comments are likely to be construed as mind games and they did not stop there, with the Argentinian - whose side are looking to retain the Copa title - praising Carlo Ancelotti's Real before Wednesday's showdown.
"You can make an argument for Madrid to be favourites in the league," he added.
"But that doesn't mean they're favourites for every game.
"When we played Madrid on match day seven (Atletico won 1-0) they had only played a few games with their new coach.
"They've grown very strong since then. They had a strong January and won many points.
"Madrid have found a system, 4-3-3, with a lot of strength at the back and speed at the front.
"We've respected the cup since we played Sant Andreu (in the club's first match of the competition) and want to get as far as possible. We continue along those same lines now."
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