Aluminum target material is an important target material and is widely used in preparations of semiconductor films, integrated circuits, display circuits, protective films, decorative films, etc. In this study, pure aluminum coatings were deposited on stainless steel substrates by cold-spray technology as part of an overall project to produce large-size pure aluminum sputtering target materials. The results show that pure aluminum coatings exhibit high adhesive strength (~98 MPa), high deposition efficiency (~95%), and low porosity (~0.3%) on stainless steel substrates. The bonding mechanisms of pure aluminum coatings on stainless steel are a combination of metallurgical and mechanical interlocking. The evolutions of microstructure and mechanical properties of pure aluminum coatings under different heat treatments were also studied. With the increase of heat treatment temperature, it is found that cold-sprayed aluminum coatings become more homogenous in microstructure, the microhardness is reduced, and the adhesive strength seems to be slightly reduced. Overall, this study demonstrates significant advantages of cold-spray technology in depositing high-performance pure aluminum coatings on stainless steels.