ABSTRACTIn this paper, the microstructural evolution and deformation mechanism of the cryorolled Fe–36%Ni alloy was investigated. Deformation twinning was confirmed to be activated at the early stage of cryorolling (CR) and subsequently suppressed due to microstructure refinement. The existence of and peaks revealed that the (α′-M) phase transformation was induced during the CR process. The stress-assisted martensite and strain-induced martensite were detected to be transformed at the grain boundary and intersection of deformation twins, respectively. Owing to the co-effect of the temperature raise and mechanical stabilisation, the α′-M phase transformation was suppressed during the CR process. Therefore, the amount of the α′-M was limited in the tested alloy.