Diego Costa's brace and a goal from Raul Garcia saw Atletico Madrid overcome Valencia 3-0 on Sunday, seeing them go level on points and goal difference with Barcelona.
But despite Atletico's brilliance in 16 league games this season, Simeone said staying in touch with Barca was too big an ask.
"Barcelona are a giant team who have an amazing record in the last decade," he said after watching his team ease past Valencia.
"(Lionel) Messi is not there, but they manage to solve their problems easily. Because they don't often struggle it is really hard to match their results. The record of Barcelona is stratospheric."
Simeone wanted more from his players against Valencia despite the three-goal win, perhaps with an eye to overtaking Barcelona at the top.
"I always want to win and obviously I always want more, so in each situation I dislike passivity and I tried to push the team in order not to be too satisfied," he said.
Simeone also spoke about Monday's UEFA Champions League draw, with his team seeded for the round of 16.
He said his side's opponents would be more experienced than his team, but believes they still have a chance of progressing.
"We know the rival we will have to face, as I already said, it is going to be tough and the tie is going to be 50-50," Simeone said.
"Every single team we could play against will have more experience than us, but I think it is going to be a 50-50 game."
