Tin-based alloys have been widely used as an excellent bearing material. However, preparing of Tin/steel bimetallic materials with sound metallurgical interfaces has proven challenging. Importantly, a large number of brittle intermetallic compounds inevitably form at the interface, affecting the material's bonding properties. In this study, an electroplated Ni layer was used for the first time as an intermediate layer in Tin/steel bimetallic composites. It solves the problems of steel surface oxidation and poor wettability. Additionally, the introduction of the electroplated Ni layer impedes the formation of brittle phases, thereby improving interfacial bond strength. The results show that the Tin/steel interface of the Ni interlayer consists mainly of a large number of Ni3Sn4 phases rather than the commonly known FeSn2 phase. A thin layer of residual Ni plating also exists between the steel and the diffusion layer. Furthermore, the properties of Ni3Sn4 and FeSn2 phases were calculated using first-principles calculations. A Tin/steel bimetallic interface achieved a maximum shear strength of 58.63 MPa in the presence of the Ni intermediate layer. At that time, the residual thickness of the Ni layer was 1.5 μm, and the thickness of the diffusion layer was 4.8 μm.