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Primal Tiger Leather can be skinned off any Ancient Tiger in the original Zul'Gurub Heroic Dungeon after earning the achievement [Relics of a Fallen Empire].
This item was found by skinning the Zulian Cubs, Zulian Tigers or the High Priest Thekal in Zul'Gurub. Both tiger types had an average chance on dropping it when skinned while the High Priest always dropped multiple pieces of Primal Tiger Leather.