In the work, an elemental mixture of Ni and Ti was deposited by atmospheric plasma spray technology on the mild steel substrate by varying the process parameters such as primary gas flow rate and plasma arc current. The properties such as surface roughness, microhardness, and erosion rate of the coating were determined and the relationship between process parameters and coating properties was established. To optimize the process parameters and to find out the optimum parametric setting, the fuzzy technique for order preference by similarity to an ideal solution hybrid technique was implemented. By keeping all the parameters constant, the coating with better properties was obtained at an optimum parametric setting of 550 A arc current and 45 lpm primary gas flow rate. Furthermore, by implementing the Analysis of Variance, the primary gas flow rate was found to be a significant contributing factor. The X-ray diffraction analysis of the coating developed at an optimized parametric setting revealed Ni, Ti, NiTi-B2 phase, Ni3Ti, Ti2Ni, Ni4Ti3, TiO, and NiO phases. The bonding of the coating with the substrate was confirmed by the line scan energy dispersive spectroscopy analysis. The surface morphology of the eroded surface of the coating developed at the optimum parameter revealed the crater formation, chip formation, lip formation, plastic deformation, and groove formation mechanisms.