A dense nanodiamond–aluminum (ND–Al) composite coating was successfully produced by low pressure cold spray (CS) deposition of ball-milled powders containing 10 wt% ND. High-energy ball milling is a feasible means for the synthesis of composite feedstock powders as it provides excellent control over particle size distribution, crystal size, and the dispersion of ND agglomerates. The resulting CS coatings were characterized with respect to deposition efficiency, particle velocity and mechanical properties. It was found that the CS deposition produced dense, ND–Al composite coatings with increases in both hardness and elastic modulus as compared to the feedstock powders. The coating hardness of the 0.5 h-milled ND–Al composite that has the highest DE (14.2%) in ND–Al composites is 3.02 GPa, an 175% increase over the pristine as-received Al (1.10 GPa). The highest elastic modulus of the composite coatings is 98.3 GPa, a 51.5% increase over the as-received Al powder.