Surface mechanical treatments are known to introduce deformation heterogeneity, thus entailing a combination of excellent strength and ductility in metallic metals. Accumulative skin pass rolling (ASPR) was employed to introduce heterogeneous structure in pure copper, which significantly improved yield strength and maintained high ductility. The experimental observations of the ASPR processed copper showed that surface grains possessed a much larger magnitude of misorientations and geometrically necessary dislocations (GNDs) than the centre grains. Crystal plasticity finite element modelling was utilised to provide an in-depth understanding of microstructure evolution during ASPR. It was found that the surface grains accommodated higher shear strain and had higher slip resistance than the centre grains. The multiple active slip systems in the surface grains induce the lattice rotations and then the formation of intragranular misorientations accompanied by a high density of GNDs, while the single active slip system in the centre grains can accommodate the applied material rotation without the lattice rotation.