He prepared for college at Ramsay Technical High School and initially attended Birmingham-Southern College, transferring to Princeton in 1937. At Princeton he majored in economics, played varsity tennis, and took his meals at Tower Club. His senior-year roommates were Pittenger, Bennett, Kobilak, and Harkness.
Following Princeton, Rolls spent six months with Bankers Trust in New York before being drafted into the Army, where he served as an officer in the Pacific theater at Eighth Army Headquarters. Returning to his native Birmingham after the war, he joined the just-formed Southern Research Institute, where he spent his entire career, retiring in 1980. In retirement Rolls golfed, studied French and traveled in France, and served on several charitable boards.
Predeceased by his wife, Allen, he is survived by his son, Rollin III of Birmingham.