Ark Royal participated in many exercises as part of the British fleet and NATO squadrons, but saw no combat duty. She was not involved in the Suez Crisis of 1956, about a year after her commissioning, because she was on her way there when she ran a main propellor shaft bearing and had to return to Devonport for a major refit. Eagle replaced her at Suez. In 1973, she carried out trials for a new type of Vertical/Short Take Off and Landing (V/STOL) aircraft, the Hawker P.1127, which later developed into the Hawker Siddeley Harrier. The same aircraft, now having been redesigned and developed as the British Aerospace Sea Harrier, was later accepted as the primary strike capability of the last Ark Royal from 1980 onwards.
She was part of the Beira Patrol enforcing the naval blockade of Rhodesia in 1965. The 1966 Defence White Paper planned the end of British carriers in the early 1970s but she went into dock for her refit to head off dockyard redundancies and the likely political issues. A new government re-examined the case for carriers finding that shore-based aircraft could not provide adequate cover for British concerns "East of Suez".
On 9 November 1970 while in the Mediterranean to participate in a NATO exercise she collided with Bravyy, a Soviet Kotlin-class destroyer which was shadowing Ark Royal (a common practice during the Cold War). Ark Royal was slightly damaged, while the Soviet destroyer sustained minor damage and two missing crew. Ark Royal??'?s commanding officer, Captain Ray Lygo, was cleared of blame at the subsequent court-martial.
The ship featured in the 1960s British television series Not Only... But Also starring Peter Cook and Dudley Moore. In one episode, they used the ship's catapult to shoot a piano into the sea. When commissions ended, items were fired off the catapult, including pianos and once a toilet complete with paying-off pennant.
By 1970, Ark Royal had a complement of 39 aircraft. This typically comprised 12 Phantom FG MK.1s, of 892 Naval Air Squadron, 14 Buccaneer S MK.2s of 809 Squadron, 4 Gannet AEW Mk.3s of B Flight 849 Squadron, 6 Sea King HAS Mk.1s of 824 Squadron, 2 Wessex HAR Mk.1s of the Ship's Flight and 1 Gannet COD Mk.4. later replaced by an AEW3. The Buccaneers doubled as tanker aircraft, using buddy refuelling pods, and as long-range reconnaissance aircraft with bomb bay-mounted camera packs. In July 1976, she represented Britain at the United States Bicentennial Celebration in Fort Lauderdale, Florida.
In 1972, the Buccaneers aboard Ark Royal took part in a long range strike mission over British Honduras shortly before its independence to deter a possible Guatemalan invasion.
In 1977, under the flag of Admiral Sir Henry Leach KCB Commander-in-Chief Fleet, Ark Royal led the Royal Navy's tribute to and celebrations of Queen Elizabeth II's Silver Jubilee at Spithead.
In the mid-1970s, the ship made a return to television. A major BBC documentary series, Sailor was made, showing life on board the ship during a February to July 1976 Western Atlantic deployment. Her commanding officer at this time was Captain Wilfred Graham, a later Flag Officer Portsmouth and the ship's Commander (executive officer) was Commander David Cowling. The theme tune for the programme was "Sailing" by Rod Stewart – a song that came to be associated with the ship and her successor. She visited Fort Lauderdale, Florida from 30 May until 14 June 1976.
She entered HMNB Devonport on 4 December 1978 and decommissioned on 14 February 1979. Like her sister Eagle, she had a relatively short (24-year) life, and when the White Ensign lowered for the last time the Royal Navy no longer had fixed wing aircraft at sea. On 29 March 1980, the Ministry of Defence (MOD) announced that she would be sold for scrap and so ended plans to preserve her. She left Devonport on 22 September 1980 under tow to be scrapped at Cairnryan near Stranraer in Scotland, arriving on the 28 September. Breaking up took until 1983. Various parts of the ship remain as souvenirs or memorials; for instance, an anchor outside the Fleet Air Arm Museum at RNAS Yeovilton.