A technology to improve the tribological and mechanical surface properties of iron alloys is developed based on the electroless nickel plating. The technology combines sol-gel and electroless deposition technique. Novel nanocomposite coatings are obtained consisting of Nickel-phosphorus-nanodiamond (Ni-P-ND). The ND sol is added directly to the electroless Ni-P solution. A suitable surfactant is added to achieve well-dispersed ND particles in the electroless solution to facilitate their embodiment and equal distribution in the coating. Substrates of steel 17CrNiMo6 and spheroidal graphite cast irons are used for the manufacture of the iron alloys specimens. The surface morphology and microstructure observation performed by scanning electron microscopy (SEM) and optical metallography confirms the influence of ND particles on the coating structure. The structural phase investigation by X Ray analysis indicates a transformation of the amorphous phase to a crystalline one such as Ni, Ni3P after coatings' heat treatment. The microhardness investigation by Knoop Method and wear resistance measurement in accordance with the Polish Standard PN-83/H-04302 of Ni-P and Ni-P-ND composite coatings are evaluated and compared with each other. The increase in the value of hardness and wear resistance of Ni-P composite coatings in the presence of ND particles and after heat treatment is obtained.