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Dilahirkan di Río Cuarto, Córdoba, Aimar began his ascent to stardom with Club Atlético River Plate, whose first team he joined for the 1997–98 season, after rejecting a place at medical school, and with whom he quickly established himself as one of the best young players in Argentina.

Valencia CF of Spain signed Aimar in January 2001, at a price of €24 million. The purchase proved justified as he helped lead the team to a first-place finish in La Liga in 2001–02 (with 33 games and four goals), as well as to a runners-up finish in the previous seasons's UEFA Champions League, being defeated by FC Bayern Munich; he also won the 2004 UEFA Cup, appearing in eight scoreless matches during the campaign – this included the final against Olympique de Marseille, where he replaced Francisco Rufete with 30 minutes to go.

On 12 April 2006 Aimar was hospitalized after being diagnosed with acute viral meningitis, but made a quick recovery and returned to play for his team. During his career with the Che, he was also often troubled with injuries.