This study evaluated the enhancement of microstructural and mechanical properties of a cross rolled Ni-10Cr alloy, comparing with conventionally rolled material. Cold rolling was carried out to 90% thickness reduction and the specimens were subsequently annealed at 700oC for 30 min to obtain a fully recrystallized microstructure. Cross roll rolling was carried out at a tilted roll mill condition of 5o from the transverse direction in the RD-TD plane. In order to observe the deformed microstructures of the cold rolled materials, transmission electron microscopy was employed. For annealed materials after rolling, in order to investigate the grain boundary characteristic distributions, an electron back-scattering diffraction technique was applied. Application of cold rolling to the Ni-10Cr alloy contributed to notable grain refinement, and consequently the average grain size was refined from 135 μm in the initial material to 9.4 and 4.2 μm in conventionally rolled and cross rolled materials, respectively, thus showing more significantly refined grains in the cross rolled material. This refined grain size led to enhanced mechanical properties such as yield and tensile strengths, with slightly higher values in the cross rolled material. Furthermore, the <111>//ND texture in the CRR material was better developed compared to that of the CR material, which contributed to enhanced mechanical properties and formability.