After starting his career with Vélez Sarsfield, Simeone moved to Italian Serie A club Pisa in 1990. The club was relegated in his first season and, after it failed to gain promotion the following year, Simeone was sold to Sevilla in the Spanish La Liga. Simeone played two seasons in Seville, after which he was signed by Atlético Madrid. At Atlético, he was part of the team which won the double of the Liga title and Copa del Rey during the 1995–96 season.