In November 1961, she sailed for her first North Atlantic deployment and operated with Antisubmarine Warfare Carrier Task Group 83.3 until February 1962.

In November 1962 she deployed to the Caribbean for support to U.S. Navy units involved in the Cuban Missile Crisis blockade effort.

In late April 1965 she was ordered south to the vicinity of the Dominican Republic to support U.S. Navy units during the crisis there and the intervention there by the U.S. Marine Corps in Operation Powerpack.

On 12 June 1965 she sailed for Northern European waters and, with other units, engaged in joint amphibious exercises with the armed forces of Norway.

Upon returning to the United States on 23 July 1965, she prepared to enter the yards for an extensive "jumboization" conversion, with preliminary work conducted at Boston, Massachusetts.

She returned to Mayport on 6 August 1968 and spent the latter part of the year servicing units of the recovery force for the Apollo 7 space mission.

Pawcatuck was stricken from the Naval Register on 21 September 1991 and was transferred to the United States Maritime Administration as part of the National Defense Reserve Fleet on the James River at Fort Eustis in Newport News, Virginia.