The performance of the Al0.5CoCrFeNi2Ti HEA atmospheric plasma-sprayed coating was extended from characterizing the properties of its powder prepared via the gas atomization method. It was observed that the gas-atomized HEA powders possessed a solid solution BCC phase, while a major phase transformation to a FCC-L21 intermetallic phase occurred during the annealing process. The formation of the intermetallic phase resulted in an increase in average hardness from 6.28 to 7.64 GPa after annealing at 900 °C for 1 h. Afterward, HEA powders were applied in the atmospheric plasma spray technology. The phase constitution of Al0.5CoCrFeNi2Ti HEA coatings was investigated by varying powder size and applied current. It was observed that the smaller powder sizes prone to oxidation, whereas higher applied current facilitated the phase transformation from BCC to FCC phase. The nanoindentation test indicated distinct average microhardness values for the interlamellar oxide region, BCC unmelted particle and FCC phase lamellar region, which was measured at 12.35, 8.68 and 5.97 GPa, respectively. As a result, the adjustability of coating hardness was achieved by manipulating the relative phase ratio.