On 21 November 1963, the squadron was renamed the Sunliners and a new insignia was approved consisting of a black background with the international orange "Sun Dial" design.

In 1958 VF-81 made a deployment as part of Air Task Group 181 (ATG-181) aboard USS Lake Champlain to the Mediterranean Sea.

The detachment was provided air cover for antisubmarine warfare units embarked on USS Essex with their AIM-9 Sidewinder missiles.

In 1969 VA-81 A-4Cs made a single deployment to the Mediterranean aboard USS John F. Kennedy as part of CVW-1, operating for a time off the coast of Libya following the 1969 Libyan coup d'état.

From July to August 1974, VA-81 operated from USS Forrestal in the vicinity of Cyprus following the coup and subsequent Turkish invasion.

VA-81 embarked on USS Forrestal from May to June 1981, operating in the eastern Mediterranean following Israeli reprisal raids against Syrian missile batteries located in southern Lebanon.

Later that night, VA-81 aircraft acted as the decoy group for VA-83's HARM strike against the Libyan missile radar site at Sirte.

On the same day, the squadron scored the Navy's only two aerial victories over enemy fighters during the campaign by downing two Iraqi MiG-21s en-route to bomb the H-3 Air Base in the western part of Iraq, by F/A-18Cs, the pilots being Nick "Mongo" Mongillo, callsign Quicksand 62, and Mark "MRT" Fox, callsign Quicksand 64.

In 2011, the squadron was embarked with CVW-17 for a Western Pacific and Persian Gulf deployment aboard USS Carl Vinson.

In 2012, the squadron completed a surge deployment with Carrier Air Wing 17 aboard USS Carl Vinson.

In 2014, the squadron was embarked with CVW-17 aboard USS Carl Vinson in support of Operation Inherent Resolve and returned to NAS Oceana in 2015.

In spring 2018, the squadron was embarked with CVW-1 aboard USS Harry S. Truman in support of Operation Inherent Resolve and returned to NAS Oceana in late summer 2018.