The present study was carried out to evaluate the microstructures and mechanical properties of severely deformed Ni-30Cr alloy. Cross-roll rolling (CRR) as severe plastic deformation (SPD) process was introduced and Ni-30Cr alloy sheets were cold rolled to a 90% thickness reduction and subsequently annealed at 700 °C for 30 min so as to obtain the recrystallized microstructure. For the analysis of grain boundary character distributions (GBCDs), electron back-scattered diffraction (EBSD) technique was introduced. CRR on Ni-30Cr alloy was effective to enhance the grain refinement through heat treatment; consequently, average grain size was significantly reduced from 33 μm in initial material to 0.6 μm in CRR processed material. This grain refinement directly affected the mechanical properties improvement, in which yield and tensile strengths were significantly increased than those of initial material. In this study, we systematically discussed the grain refinement, accompanying with increase in mechanical properties, in terms of the effective strain imposed by CRR, comparing with conventional rolling (CR).