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Ni-free and Ni-bearing steels were designed to elucidate the effect of Ni on the free energy of bainitic transformation. Steels with two distinct nano-bainite structures were obtained through conventional one-stage and two-stage isothermal treatments. The effect of work hardening and accompanying strain on martensitic transformation of the two nano-bainite structures was also studied. Microstructure of both the steels consisted of bainitic ferrite and film-like and block-like retained austenite (RA). The total carbon concentration, degree of Fe–C cluster formation, and stability of RA were significantly affected by the free energy of bainitic transformation. The presence of Ni leads to reduction in the free energy of bainitic transformation, refinement of bainite structure, and extension of bainite nucleation regime. The carbon-content in block-like and film-like RA microstructure of Ni-bearing steel was 5.5% and 19.1%, respectively, which was greater than Ni-free steel. The load-displacement behavior indicated superior strain hardenability and higher strain hardening rate (SHR) in Ni-bearing steel. The uniform nanostructure of Ni-bearing steel promoted the formation of stable film-like RA between bainitic ferrite, leading to higher strain hardening rate and stronger transformation-induced plasticity (TRIP) effect at large strain. The Ni-bearing steel was characterized by superior plasticity (13.7%–10.3%) and product of tensile strength and % elongation (25.9 GPa·% to 20.9 GPa·%) in comparision to the Ni-free steel. [ABSTRACT FROM AUTHOR]