With her home port at Norfolk, Virginia, Ray underwent shakedown training and weapons and sonar testing until 6 October 1967, when she deployed to conduct Atlantic Ocean submarine operations until 12 December 1967.

After its completion, she departed Norfolk on 5 March 1972 and engaged in various tests and exercises—notably two North Atlantic Treaty Organization exercises, "Strong Express" and "Escort Deep"—during the remainder of 1972.

After the overhaul the Ray went to New London CT for refresher training and then for a month in the Caribbean (Puerto Rico and St. Croix) for shakedown and sonar calibration.

On 20 September 1977 Ray struck a coral mountain while submerged in the Mediterranean Sea 10 miles (16 km) off the coast of Tunisia due to a combination of equipment failure and crew inexperience.

Ray participated in a six-month Mediterranean cruise as a part of the USS Forrestal (CVA-59) aircraft carrier battle group from October 1989 to April 1990.

Her scrapping via the Nuclear-Powered Ship and Submarine Recycling Program at Puget Sound Naval Shipyard at Bremerton, Washington, began on 15 March 2002 and was completed on 30 July 2003.