The unique flash heating characteristics of intense pulsed ion beams (IPIB) offer potential advantages to fabricate high-performance coatings with non-equilibrium structures. In this study, titanium-chromium (Ti-Cr) alloy coatings are prepared through magnetron sputtering and successive IPIB irradiation, and the feasibility of IPIB melt mixing (IPIBMM) for a film-substrate system is verified via finite elements analysis. The experimental results reveal that the melting depth is 1.15 μm under IPIB irradiation, which is in close agreement with the calculation value (1.18 μm). The film and substrate form a Ti-Cr alloy coating by IPIBMM. The coating has a continuous gradient composition distribution, metallurgically bonding on the Ti substrate via IPIBMM. Increasing the IPIB pulse number leads to more complete element mixing and the elimination of surface cracks and craters. Additionally, the IPIB irradiation induces the formation of supersaturated solid solutions, lattice transition, and preferred orientation change, contributing to an increase in hardness and a decrease in elastic modulus with continuous irradiation. Notably, the coating treated with 20 pulses demonstrates a remarkable hardness (4.8 GPa), more than twice that of pure Ti, and a lower elastic modulus (100.3 GPa), 20% less than that of pure Ti. The analysis of the load-displacement curves and H-E ratios indicates that the Ti-Cr alloy coated samples exhibit better plasticity and wear resistance compared to pure Ti. Specifically, the coating formed after 20 pulses exhibits exceptional wear resistance, as demonstrated by its H3/E2 value being 14 times higher than that of pure Ti. This development provides an efficient and eco-friendly method for designing robust-adhesion coatings with specific structures, which can be extended to various bi- or multi-element material systems.