In this paper, four kinds of Ni-xCr alloy cladding layers (x=20wt%, 40wt%, 60wt% and 80wt%) were prepared by high-speed laser cladding technology, and the relationship between microstructure and wear resistance of Ni-Cr alloy cladding layers with different Cr contents was investigated. The results showed that the organizations of the four Ni-Cr alloy cladding layers were all of reticulated dendritic structure. Among them, Ni-20Cr and Ni-40Cr are single-phase γ-(Ni,Cr) solid solutions, and their wear mechanisms are adhesive wear and abrasive wear. With the increase of Cr content, Ni-60Cr and Ni-80Cr are γ-(Ni,Cr) phase and Cr phase, and Cr-rich precipitates also appear, and the wear mechanism is adhesive wear, abrasive wear and fatigue wear. A moderate increase in Cr content can enhance the hardness and wear resistance of Ni-Cr alloy cladding layer. However, excessive addition of Cr results in the precipitation of Cr-rich precipitates. The hardness of these precipitates is 248 HV0.1, which is lower than the hardness of the Ni-60Cr matrix (410.7 HV0.1) and Ni-80Cr matrix (716.6 HV0.1). A hardness transition zone exists between the Cr-rich precipitates and the matrix. Cracks are likely to form and expand in this zone, leading to deep spalling, which is not conducive to the wear-resistant properties of the cladding layer. Ni-80Cr has the highest hardness, but its high Cr content leads to a large number of penetrating cracks and a high number of Cr-rich precipitates on the surface, ultimately resulting in the worst wear resistance. On the other hand, Ni-60Cr exhibits the best wear resistance due to its high hardness and dense microstructure.