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This paper reports the effect of the processing route on the microstructure and mechanical properties in the pure copper sheets processed by single-roll angular-rolling (SRAR). The SRAR process was repeated up to six passes in two processing routes, called routes A and C in equal-channel angular pressing. As the number of passes increased, the heterogeneous evolution of hardness and microstructural heterogeneities between the core and surface regions gradually became intensified in both processing routes. In particular, route A exhibited more prominent partial grain refinement and dislocation localization on the core region than route C. The finite element analysis revealed that the intense microstructural heterogeneities observed in route A were attributed to effective shear strain partitioning between the core and surface regions by the absence of redundant strain. On the other hand, route C induced reverse shearing and cancellation of shear strain over the entire thickness, leading to weak shear strain partitioning and delayed grain refinement. Ultimately, this work suggests that route A is the preferred option to manufacture reverse gradient structures in that the degree of shear strain partitioning and microstructural heterogeneity between the core and surface regions is more efficiently intensified with increasing the number of passes.