Aluminum-copper alloy system is extensively used in structural and aerospace applications for its high strength-to-weight ratio, good mechanical and tribological properties. Improving the properties of these alloys would likely widen their application area. In the present work, an attempt has been made to simultaneously enhance the wear resistance and mechanical properties of an Al-Cu alloy, AA2014 by imparting different levels of cryorolling strains and postroll aging treatment. The wear behavior of the material is studied under dry sliding condition by pin-on-disk experiments and mechanical properties are assessed by tensile test. Formation of high fraction of dislocation density and significant refinement of microstructure during cryorolling and nucleation of fine coherent Guinier-Preston (GP) zones of Al2Cu precipitates during postcryoroll aging has led to about 100% increment in the wear resistance of the material. Tensile test results proved that the synergetic effect of cryorolling and aging treatment led to 53% increment in strength (557 MPa) without compromising the material's ductility (22.5%). A detailed investigation on the various mechanisms responsible for the enhanced wear resistance and improved mechanical performance is presented based on the microstructural evidence. © 2018 by ASME.