Laser surfacing in the form of cladding, alloying, and modifications are gaining widespread use because of its ability to provide high deposition rates, low thermal distortion, and refined microstructure due to high solidification rates. Because of these advantages, laser surface alloying is considered a prime candidate for producing ultra-hard coatings through the establishment or in situ formation of composite structures. Therefore, a program was conducted by the Applied Research Laboratory, Pennsylvania State University and Oak Ridge National Laboratory to develop the scientific and engineering basis for performing laser-based surface modifications involving the addition of hard particles, such as carbides, borides, and nitrides, within a metallic matrix for improved wear, fatigue, creep, and corrosion resistance. This has involved the development of advanced laser processing and simulation techniques, along with the refinement and application of these techniques for predicting and selecting materials and processing parameters for the creation of new surfaces having improved properties over current coating technologies. This program has also resulted in the formulation of process and material simulation tools capable of examining the potential for the formation and retention of composite coatings and deposits produced using laser processing techniques, as well as positive laboratory demonstrations in producing these coatings. In conjunction with the process simulation techniques, the application of computational thermodynamic and kinetic models to design laser surface alloying materials was demonstrated and resulted in a vast improvement in the formulation of materials used for producing composite coatings. The methodology was used to identify materials and to selectively modify microstructures for increasing hardness of deposits produced by the laser surface alloying process. Computational thermodynamic calculations indicated that it was possible to induce the precipitation of titanium carbonitrides during laser surface alloying provided there was sufficient amount of dissolved titanium, carbon, and nitrogen in the liquid steel. This was confirmed experimentally by using a powder mixture of 431-martensitic steel, titanium carbide powder, and nitrogen shielding, during laser deposition to produce deposits exhibiting relatively high hardness (average surface hardness of 724 HV). The same approach was extended to direct diode laser processing and similar microstructures were attained. The above analysis was extended to develop an in-situ precipitation of Ti(CN) during laser deposition. The Ti addition was achieving by mixing the 431 martensitic steel powders with ferro-titanium. The dissolution of nitrogen was achieved by using 100% nitrogen shielding gas, which was indicated by thermodynamic analysis. Demonstrations were also conducted utilizing the tools developed during the program and resulted in several viable composite coating systems being identified. This included the use of TiC and ferro-titanium in martensitic-grade stainless steel matrix material with and without the use of active N2 shielding gas, WC hard particles in a martensitic-grade stainless steel matrix material, WC and BN in a nickel-based matrix material, and WC in highly alloyed iron-based matrix. Although these demonstrations indicated the potential of forming composite coatings, in certain instances, the intended industrial applications involved unique requirements, such as coating of internal surfaces, which hindered the full development of the improved coating technology. However, it is believed that the addition of common hard particles, such as WC or TiC, to matrix material representing martensitic grades of stainless steel offer opportunities for improved performance at relatively low material cost.