Metallization of Carbon Fiber-Reinforced Polymer (CFRP) composites aggrandized their application to aircraft, automobile, and wind power industries. Recently, the metallization of CFRP surface using thermal spray technique, especially the cold spray, a solid state deposition technique, is a topic of research. However, a direct cold spray deposition on the CFRP substrate often imposes severe erosion on the surface owing to the high-impact energy of the sprayed particles. This urges the requirement of an interlayer on the CFRP surface. In the present study, the effect of surface treatment on the interlayer adhesion strength is evaluated. The CFRP samples were initially treated mechanically, chemically, and thermally and then an interlayer was developed by atmospheric plasma spray system. The quality of the coating is highly dependent on the splat taxonomy; therefore the present work also devoted to study the splat formation behavior using the splat-collection experiments, where the molten Cu particles impinged on the treated CFRP substrates. These results were correlated with the coating adhesion strength. The coating adhesion strength was measured by pull-out test. The results showed that the surface treatment, particularly the chemical treatment, was fairly successful in improving the adhesion strength.