The cladding process using laser beam radiation comprises different operational regimes, depending on the involved lasers (usually CO2 or Nd:YAG) and materials. A series of experiments has been carried out to investigate Nd:YAG laser cladding using MoSi2 powder. Procedures and operating parameters for producing clad layers has been developed and their properties evaluated. The feasibility of the laser cladding technique, using a high power Nd:YAG laser, by projecting MoSi2 powder on steel substrate was demonstrated. The results indicate a low density of cracks, elevated powder catchment efficiency (between 65 and 90%) and hardness values around 1200–1300 HV. Our goal consists in crack reduction (ideally elimination) and to reach that we have considered the addition of components that can create opposing stresses during solidification, like non-stabilized Zirconia powder particles. The results of these experiments are also widely presented in the paper.