He played as an amateur from 1950 on, before he was active as a professional from 1962 until his retirement. In singles he reached the final of the French Open in 1958 and 1960 , but lost to Mervyn Rose in three and Nicola Pietrangeli in five sets. As early as 1956 he was able to win the mixed doubles at the French Open alongside Thelma Coyne Long .
Between 1952 and 1960 Luis Ayala completed 18 games for the Chilean Davis Cup team . He won 27 of his 33 singles and 10 of his 18 doubles games. This makes him the player with the most individual wins and the most wins overall in Chilean Davis Cup history.