The contract to build Casimir Pulaski was awarded to the Electric Boat Division (EB) of the General Dynamics Corporation in Groton, Connecticut, on 20 July 1961 and her keel was laid down there on 12 January 1963.

[2] After she was commissioned on 14 August 1964,[2] Casimir Pulaski stood out of Electric Boat for a three-month shakedown cruise with both crews to the waters off Cape Kennedy where she test-fired multiple UGM-27 Polaris ballistic missiles.

[2] After completing 20 deterrent patrols, Casimir Pulaski returned to EB in Groton, Connecticut on 5 January 1970 for refueling and overhaul where the S5W reactor was replaced with an S3G core 3 and the boat became the seventh SSBN refitted to carry UGM-73 Poseidon ballistic missiles.

[3] In June 1971, while in Holy Loch, Casimir Pulaski was the first boat to have the Integrated Data Acquisition System (IDAS) M-35 set installed.

From 1 April to 20 May 1989, Casimir Pulaski participated in Concept of Operation Exercise LANTCOOPEX 1-89, held at a remote site—Port Canaveral—away from an SSBN refit port, arriving there after the end of Gold Crew deterrent patrol.

In November, the Blue Crew sailors were awarded the Humanitarian Service Medal for their actions in response to Hurricane Hugo which caused widespread damage in the Caribbean and the southeast United States.

After her final cruise under Commander Kenneth W. Wrona, Casimir Pulaski was decommissioned on 7 March 1994 and simultaneously stricken from the Naval Vessel Register.