Physical, optical, and mechanical properties of silicon carbonitride (a‐SiCN) films produced by remote hydrogen plasma chemical vapor deposition (RP‐CVD) using aminosilane and disilazane precursors are examined in relation to their chemical structure. The films deposited at different temperatures (30–400°C) were characterized in terms of their density, refractive index, optical bandgap, photoluminescence, adhesion to a substrate, hardness, elastic modulus resistance to wear (predicted from the “plasticity index” values), and friction coefficient. Reasonable structural dependencies of film properties were determined using the relative integrated intensities of the infrared absorption bands from the Si−N and Si−C bonds, and the X‐ray photoelectron spectroscopy Si2p band from the Si−C bonds (controlled by substrate temperature) evaluated in the first part of this study. In view of their good mechanical properties, a‐SiCN films seem to be useful coatings for improving surface mechanics of engineering materials for advanced technology.