A typical trade-off relationship exists between strength and elongation in face-centered cubic metals. Studies have recently been conducted to enhance strength without ductility reduction through surface-treatment-based ultrasonic nanocrystalline surface modification (UNSM), which creates a gradient microstructure in which grains become smaller from the inside to the surface. The transformation-induced plasticity effect in Fe-Mn alloys results in excellent strength and ductility due to their high work-hardening rate. This rate is achieved through strain-induced martensitic transformation when an alloy is plastically deformed. In this study, Fe-6%Mn powders with different sizes were prepared by high-energy ball milling and sintered through spark plasma sintering to produce Fe-6%Mn samples. A gradient microstructure was obtained by stacking the different-sized powders to achieve similar effects as those derived from UNSM. A compressive test was performed to investigate the mechanical properties, including the yielding behavior. The deformed microstructure was observed through electron backscatter diffraction to determine the effects of gradient plastic deformation.