The development of graded microstructure in Ni-base Alloy 602CA, processed through the new technique of high reduction (per pass) cold rolling (HRCR) and the severe surface plastic deformation technique of ultrasonic nanocrystal surface modification (UNSM) was investigated. Clear through-thickness gradients in residual stress, dislocation structure and boundary density with misorientation >2° were observed after the HRCR and UNSM. However, the gradient in HRCR did depend on the roll-pass schedule: relative reduction per pass, total reduction and direction of the roll pass. Applying maximum reduction per pass and minimum number of passes exhibited an improved graded microstructure for 40% total reduction in both unidirectional (UR) and cross rolling (CR) cases. The UR40 and CR40 in HRCR process led to graded microstructures that compared well with those produced by UNSM. © 2019 Elsevier Inc.