High-velocity oxy-fuel (HVOF)-sprayed coatings have performed exceptionally well in low-energy particle impact wear and are accepted worldwide. However, their application for high-energy particle impact wear (HEPIW) requires a different approach and more efforts. HVOF-coating systems typically use WC-Co, WC-Co-Cr, WC-Ni-Cr, and FeCrAlY-Cr3C2 powders. WC-Co-Cr powders are preferred when there is a high demand for corrosion resistance. WC-10Co-4Cr coating powder has been selected in the current study. To improve coating properties such as microhardness, fracture toughness, and HEPIW resistance, a new approach of surface treatment with robotically controlled high-power diode laser (HPDL) is attempted. The robotically controlled HVOF-coating deposition and laser surface treatment were monitored using real-time diagnostic control. The HPDL-treated coating has been compared with “as-sprayed” HVOF coating for HEPIW resistance, fracture toughness, microhardness and microstructure. The coating characteristics and properties after laser surface treatment have improved many times compared with “as-sprayed” HVOF coating. This is due to the elimination of pores in the coating and formation of a metallurgical bond between coating and substrate. This new development opens up a possibility of using such laser treatments in specialized areas where HEPIW damages are acute. The fracture toughness and HEPIW resistance along with optical micrographs of HPDL-treated and untreated HVOF coatings are discussed and reported in this article. HEPIW resistance is observed to be proportional to the product of fracture toughness and microhardness of the HVOF coating.