As an industrial solid waste, the original aluminum ash (OAA) will cause serious pollution to the air and soil. How to reuse the OAA has been a research difficulty. Thus, a method of preparing a plasma spray powder using OAA is proposed. The OAA was hydrolyzed and ball milled, and the flowability of original aluminum ash spray powder (OAASP) was evaluated by the angle of repose. The coating properties were determined via analyzing the microstructure and the phase of the coating, and the effects of plasma spray parameters on the coating properties were investigated by the orthogonal experiment to optimize spray parameters. The results show that the angle of repose of OAASP after granulation was less than 40°, which met the requirements of plasma spraying. When the spraying current was 600 A, the spraying voltage was 60 V, the main gas flow was 33 slpm, and the powder flow rate was 22 g/min, and the prepared original aluminum ash coating (OAAC) had excellent comprehensive performance. After the spraying process parameters were optimized, the microhardness of the coating was 606.54 HV, which is about twice the hardness of the substrate; the abrasion rate was 12.86 × 10−3 g/min; the porosity was 0.16%; and the adhesive strength was 16 MPa. When the amount of Al2O3 added was 50%, the hardness of the coating was increased by 17.61%.