We elucidate here the fundamental principles underlying the modulation of osteoblasts functions in stainless steel biomedical devices achieved by nanoscale/submicron grain structure obtained through the novel concept of phase reversion in a low Ni bearing 15Cr–9Mn–1.7Cu steel. Interestingly, a comparative investigation of nano/submicron (N-SM) and coarse-grained (CG) structure under identical conditions indicated that cell attachment, proliferation, and viability are favorably enhanced in N-SM grained structure and significantly different from the CG structure. These observations were further confirmed by expression levels of vinculin and associated actin cytoskeleton. Computational analysis of immunofluorescence micrographs suggested increased vinculin concentration associated with actin stress fibers in the outer regions of the cells and cellular extensions, implying enhanced cell–substrate interactions on the N-SM grained substrate. The favorable enhancement of osteoblasts functions and cellular attachment on N-SM grained surface is attributed to ultrafine grain size, i.e., the availability of greater open lattice in the position of high angle grain boundaries, and high hydrophilicity. The integration of cellular and molecular biology with material science and engineering as described here provides a route to modulate cellular and molecular reactions in promoting osteoinductive signaling of surface adherent cells. The end outcome of the study is that stainless steels with low Ni contents in comparison to the conventionally used bioimplant with 10–13 wt%Ni, as specially processed, exhibit desired, enhanced cell functions, and bulk properties.