At the time of commissioning, Sylvania was the second of a new class of combat store ship designed to combine the functions of the AF (store ship), AKS (stores issue ship), and AVS (aviation issue ship).
 She completed fitting out and, after sea trials, departed California for duty with the Atlantic Fleet.
 The Panama Canal was transited on 11 August, and the ship arrived at Norfolk on 16 October 1964 for post-shakedown availability.
 Upon completion of this, the ship operated in the Norfolk area until the spring of 1965.

Sylvania stood out of Norfolk on 14 April 1965, en route to the Mediterranean and her first tour of duty with the 6th Fleet.
 She called at Rota, Spain, and arrived at her new home port, Naples, Italy, on 29 April.
Two days later, she began her first underway replenishment operation with the 6th Fleet.
 On 31 July, Sylvania completed the first vertical replenishment of an aircraft carrier using UH-46A helicopters.
 In early October the store ship logged her 1,000th accident-free helicopter landing.
 She served as flagship for the Service Force, 6th Fleet, from 5 December 1966 to 17 April 1967.
 During the night of 8 January 1968, the cargo ship suffered her only material loss of the year.
 She experienced a roll of 38 degrees and took water over the flight deck.
 The roll, wind, and water parted the tie-downs on cargo staged on the flight deck for the next day's replenishment.
 Consequently, 52 pallets of provisions were lost.
 On 1 July 1968, Sylvania was awarded the Battle Efficiency "E" for her class and the Supply "E" for Supply Efficiency.
 She also won the Marjorie Sterrett Battleship Fund Award for the Atlantic Fleet.

As part of Task Force 60 and as independently directed by COMSIXTHFLT, Sylvania came to the assistance of USS Liberty on 8 June 1967 when she suffered an unprovoked attack by Israeli naval and air forces during the six day Arab-Israel war.
<1537Z08 June 1967 drafted message text from
Commander, Sixth Fleet to U.S.S. Sylvania>
Sylvania was honored on 19 October by a visit from the Assistant Secretary of the Navy, Charles A. Bowser, and a party of eight who came aboard for a briefing and tour and to observe an underway replenishment exercise.
 The ship was in drydock at Malta from 29 November until 10 December 1968 when she returned to normal 6th Fleet operations.
 On 16 June 1969 the ship lost a UH-46D helicopter when it crashed during vertical replenishment operations in the harbor of Palma de Mallorca, but the crew was rescued.
 On 30 September, the ship left the 6th Fleet and returned to Norfolk on 24 October after an absence of four and one-half years.
At the time of commissioning, Sylvania was the second of a new class of combat store ship designed to combine the functions of the AF (store ship), AKS (stores issue ship), and AVS (aviation issue ship).  She completed fitting out and, after sea trials, departed California for duty with the Atlantic Fleet.  The Panama Canal was transited on 11 August, and the ship arrived at Norfolk on 16 October 1964 for post-shakedown availability.  Upon completion of this, the ship operated in the Norfolk area until the spring of 1965.
Sylvania stood out of Norfolk on 14 April 1965, en route to the Mediterranean and her first tour of duty with the 6th Fleet.  She called at Rota, Spain, and arrived at her new home port, Naples, Italy, on 29 April. Two days later, she began her first underway replenishment operation with the 6th Fleet.  On 31 July, Sylvania completed the first vertical replenishment of an aircraft carrier using UH-46A helicopters.  In early October the store ship logged her 1,000th accident-free helicopter landing.  She served as flagship for the Service Force, 6th Fleet, from 5 December 1966 to 17 April 1967.  During the night of 8 January 1968, the cargo ship suffered her only material loss of the year.  She experienced a roll of 38 degrees and took water over the flight deck.  The roll, wind, and water parted the tie-downs on cargo staged on the flight deck for the next day's replenishment.  Consequently, 52 pallets of provisions were lost.  On 1 July 1968, Sylvania was awarded the Battle Efficiency "E" for her class and the Supply "E" for Supply Efficiency.  She also won the Marjorie Sterrett Battleship Fund Award for the Atlantic Fleet.
As part of Task Force 60 and as independently directed by COMSIXTHFLT, Sylvania came to the assistance of USS Liberty on 8 June 1967 when she suffered an unprovoked attack by Israeli naval and air forces during the six day Arab-Israel war. <1537Z08 June 1967 drafted message text from
Commander, Sixth Fleet to U.S.S. Sylvania>
Sylvania was honored on 19 October by a visit from the Assistant Secretary of the Navy, Charles A. Bowser, and a party of eight who came aboard for a briefing and tour and to observe an underway replenishment exercise.  The ship was in drydock at Malta from 29 November until 10 December 1968 when she returned to normal 6th Fleet operations.  On 16 June 1969 the ship lost a UH-46D helicopter when it crashed during vertical replenishment operations in the harbor of Palma de Mallorca, but the crew was rescued.  On 30 September, the ship left the 6th Fleet and returned to Norfolk on 24 October after an absence of four and one-half years.
USS Sylvania (AFS-2)