This research investigates the potential of pulsed laser deposition to create reliable high current ohmic contacts of Ni2Si on single crystal 4H-SiC. Since this stoichiometry is the stable interphase in the nickel-silicon carbide diffusion couple, direct deposition eliminates the detrimental excess carbon normally formed by direct sintering Ni on SiC, the surface roughening that results from this sintering as well as the need for post-deposition high-temperature (900°C) anneals that are required in complex multi-component contacts. This study examines the processing parameters that must be used during deposition to obtain the desired microstructural characteristics for the contact. Pulsed laser deposition of nickel silicide produces smooth films with an amorphous or nanocrystalline structure interspersed with macroparticles. Macroparticle formation on the resulting films appear in the form of solidified droplets of the eutectic composition nickel silicide (3:1) that form during the long term target processing. The dependence of the number and size distributions of these droplets on laser fluence sample temperature is examined.