In this study, the bond–slip behavior between a new type of M-section steel skeleton (i.e., M-section steel) applied in assembled shear wall structures and concrete was investigated. First, push-out tests were conducted on 21 M-section steel–concrete (MSSC) specimens, wherein the effects of the concrete cover, concrete strength, and anchorage length on the bond strength between the M-section steel and concrete were considered. Further, the crack patterns, strain distribution of M-section steel, and bond–slip curves of the MSSC specimens were investigated using conventional strain measurement and a non-contact optical three-dimensional deformation measurement system, Digital Image Correlation–3D (DIC-3D). The experimental results demonstrated that the bond–slip curves of the MSSC specimens were divided into four stages: the linear ascending, non-linear ascending, non-linear descending, and residual stages. The initial average bond strength was mainly affected by the concrete strength and anchorage length, whereas the concrete cover and anchorage length influenced the residual average bond strength , and the ultimate average bond strength was affected by the concrete strength, concrete cover, and anchorage length. Consequently, a bond–slip constitutive model of M-section steel and concrete was proposed based on the experimental results, and consistency was observed in comparison with the test results, which verified the applicability of the proposed model. Furthermore, to verify the rationality of the bond–slip constitutive model, a numerical simulation was performed, wherein the bond–slip curves, stress clouds, and interfacial bond damage process of the MSSC specimens were investigated. The numerical simulation results indicated that the bond–slip constitutive model could accurately predict the entire failure process of the MSSC specimens.