The contract to build Grayling was awarded on 5 September 1962 and her keel was laid down at the Portsmouth Naval Shipyard at Kittery, Maine, on 12 May 1964.

She was launched on 22 June 1967, sponsored by Miss Lori Brinker, the daughter of Lieutenant Commander Robert Brinker, who was commanding officer of the previous Grayling (SS-209) when she was lost with all hands in September 1943 during World War II.

[4] In June 1996, Grayling took part in Exercise TAPON 96,[5] a North Atlantic Treaty Organization exercise held in the Alboran Sea, Gulf of Cadiz, and eastern Atlantic Ocean, along with the U.S. Navy destroyer USS Conolly, the Spanish aircraft carrier Príncipe de Asturias, the Spanish frigates Baleares, Santa María, and Numancia, the Spanish submarine Delfin, and the Greek destroyer Formion.

Grayling was deactivated on 1 March 1997, placed in commission in reserve a week later as she entered the Ship and Submarine Recycling Program, then decommissioned and stricken from the Naval Vessel Register on 18 July 1997.

Her scrapping via the U.S. Navy's Ship and Submarine Recycling Program at Puget Sound Naval Shipyard at Bremerton, Washington, was completed on 31 March 1998.