The present study was carried out to evaluate the microstructural and mechanical properties of cross-roll rolled pure copper sheets, and the results were compared with those obtained for conventionally rolled sheets. For this work, pure copper (99.99 mass%) sheets with thickness of 5 mm were prepared as the starting material. The sheets were cold rolled to 90% thickness reduction and subsequently annealed at 400˚C for 30 min. Also, to analyze the grain boundary character distributions (GBCDs) on the materials, the electron back-scattered diffraction (EBSD) technique was introduced. The resulting cold-rolled and annealed sheets had considerably finer grains than the initial sheets with an average size of 100 μM. In particular, the average grain size became smaller by cross-roll rolling (6.5 μM) than by conventional rolling (9.8 μM). These grain refinements directly led to enhanced mechanical properties such as Vickers micro-hardness and tensile strength, and thus the values showed greater increases upon cross-roll rolling process than after conventional rolling. Furthermore, the texture development of<112>//ND in the cross-roll rolling processed material provided greater enhancement of mechanical properties relative to the case of the conventional rolling processed material. In the present study, we systematically discuss the enhancement of mechanical properties in terms of grain refinement and texture distribution developed by the different rolling processes.