Engineering nanostructures in metallic materials such as nanograins and nanotwins can promote plastic performance significantly. Nano/ultrafine-grained metals embedded in coarse grains called bimodal metals and nanotwinned polycrystalline metals have been proved to possess extensively improved yield strength whilst keeping good ductility. This paper will present an experimental study on nanostructured stainless steel prepared by surface mechanical attrition treatment (SMAT) with surface impacts of lower strain rate (10 s−1–103 s−1) and higher strain rate (104 s−1–105 s−1). Microstructure transition has been observed from the original γ-austenite coarse grains to α′-martensite nanograins with bimodal grain size distribution for lower strain rates to nanotwins in the ultrafine/coarse grained austenite phase for higher strain rates. Meanwhile, we will further address the mechanism-based plastic models to describe the yield strength, strain hardening and ductility in nanostructured metals with bimodal grain size distribution and nanotwinned polycrystalline metals. The proposed theoretical models can comprehensively describe the plastic deformation in these two kinds of nanostructured metals and excellent agreement is achieved between the numerical and experimental results. These models can be utilized to optimize the strength and ductility in nanostructured metals by controlling the size and distribution of nanostructures.