<p>A comprehensive study of effect of cold spray parameters on the deposition efficiency and composition of Ni/Al mixtures was carried out. Nickel and aluminum powders were mixed in atomic ratios of 20:80, 40:60, 60:40, and 80:20. Cold spraying was carried out on aluminum substrate using N₂ gas at various gas pressures of 3, 5, and 6&#xa0;MPa, and gas temperatures of 400&#xa0;°C, 500&#xa0;°C, and 600&#xa0;°C. The effect of cold spray process parameters and feedstock composition on the composition of the coating and the overall deposition efficiency (DE) was analyzed. Higher gas temperature and pressure increased the velocity of the particles, improving the overall DE of the feed powders. Higher amount of nickel in the feed mixture resulted in reduction of overall DE. Maximum deposition efficiency of 96 and 86.5 pct was observed for 20:80 and 80:20 mixtures, respectively, for 6&#xa0;MPa and 600&#xa0;°C spray condition. The Ni₄₀Al₆₀ mixture resulted in coating compositions closer to NiAl phase range for all the process conditions. The XRD patterns indicated no new phase formation in the coatings, and the calculated composition from XRD intensities matched with the image analysis results. The hardness of the coatings increased with nickel content following an iso-stress prediction and the gas pressure and temperature had less effect. The correlation between the deposition efficiency and coating composition with the cold spray parameters and composition of the powder was analyzed using response surface methods (RSM) assisted by analysis of variance (ANOVA). <i>F</i>-test and sum of squares (SS) studies were performed to understand the significance of the cold spray parameters on the final coating.</p>