Gradient induced unusual strain hardening achieves the equilibrium of the strength and plasticity of alloys, and is an important strategy for the optimization of the mechanical properties of metals and alloys. The segregation of solute elements can greatly improve the grain boundary stability, inhibit grain coarsening and promote the mechanical strength of the alloy. In our efforts, the segregation structure of the solute element Co was designed and added to the gradient nano Ni-Co alloy, and the two strengthening strategies were applied simultaneously in one structure. The mechanical strength of the alloy achieved a second increase based on the unique combination of gradient induced strain hardening and high plasticity, especially the yield strength of alloy increase amplitude reach to 42%. This provides a positive direction for the alloy strengthening strategy. In the process of secondary strengthening, the micro-mechanism is divided into two stages: in the first stage, the gradient strain provides the alloy with geometrically necessary dislocations and a multi-axial stress state, and the existence of large numbers of geometrically necessary dislocations creates good conditions for the second stage strengthening. In the second stage, the solute segregation induced stable grain boundaries produce a strong pinning effect on the geometrically necessary dislocation, which realizes the coupling of grain boundary strengthening and dislocation strengthening. This provides a new strengthening strategy and positive theoretical guidance for the experimental preparation of advanced alloys with excellent properties.