El Cholo had previously played down his side’s chances of claiming the title - despite Atletico moving top of the table on Sunday.
“I insist. I don’t think we can win the League,” he told reporters prior to Wednesday’s Copa del Rey Madrid derby.
“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.”
Cup holders Atleti travel to the Santiago Bernabeu for the first-leg of the semi-final on Wednesday evening and Simeone accepts that while Madrid may be among the favourites to win the League, it doesn’t work that way in an individual game.
“You can make an argument for Madrid to be favourites in the League,” Simeone said.
“But that doesn’t mean they’re favourites for every game.”
Simeone - who refused to be drawn into the debate over Cristiano Ronaldo’s red card - added that the Cup is as important as ever to his side.
“We’ve respected the Cup since we played Sant Andreu and want to get as far as possible.
“We continue along those same lines now.”
Simeone revealed that Tiago could be involved against Madrid and praised Madrid for their recent form.
“When we played Madrid on match day seven 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.”
Simeone also offered kind words towards Iker Casillas, who is likely to be in goal for Madrid.
“Iker is a great ‘keeper and has made history with the national team and Madrid.
“He has performed when he has had to play and it’s especially hard when you’ve not played for a while.”
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