The Angels hired Baylor on Wednesday to replace Jim Eppard, who wasn't retained by manager Mike Scioscia.
The 64-year-old Baylor had been Arizona's hitting coach for the past three years. He is the former manager of the Rockies and Cubs.
Baylor won the AL MVP award while playing for the Angels in 1979, batting .296 with 36 homers and 139 RBIs.
He spent six seasons with the then-California Angels, hitting 141 homers.
Eppard and bench coach Rob Picciolo were let go by the Angels last week when the club confirmed Scioscia and general manager Jerry Dipoto were staying. Third base coach Dino Ebel was promoted to bench coach.