Simeone won the 1991 and 1993 editions of the Copa América with Argentina. He played in the 1994, 1998, and 2002 FIFA World Cups. He was a member of the team that won the silver medal at the 1996 Summer Olympics in Atlanta, Georgia, as one of the three over-23 players allowed per squad. As a midfielder, Simeone scored 11 goals for his country, including one in the final of the 1992 King Fahd Cup.