"Don passed from this earth with the same fierce dignity with which he played the game and lived his life," his wife, Rebecca, said in a statement.
Baylor was diagnosed with multiple myeloma 14 years ago, his family said.
Baylor managed the Cubs from 2000 to 2002. He was fired mid-season in 2002 after compiling a record of 187-220 with the Cubs.
Baylor also played 19 seasons for the Orioles, Athletics, Angels, Yankees, Red Sox and Twins, winning the 1979 MVP while a member of the Angels. He batted .260 with 338 home runs and 1276 RBIs.