TiCrCN coatings were sprayed by mixing aggregated Ti-graphite powders and metallic Cr powders with different weight ratios. The microstructure and surface crystallization behavior were researched. The results confirmed that the phases in the TiCN coating were TiC0.7N0.3 + TiC0.8 N0.2 + Ti3O + CNx + graphite (unreacted). In contrast, the TiCrCN coating included metallic Cr and TiCrCN in addition to TiC0.7N0.3, TiC0.8N0.2, Ti3O, CNx, and unreacted graphite. With the increase of Cr, the content of Cr phase increased, coupling with TiC0.7N0.3 and Ti3O decreasing. The addition of Cr decreased the cracks and pores in the sprayed TiCN and TiCrCN coatings, and changed the surface crystallization behavior from dendritic crystals to columnar crystals.