Electroless nickel (EN) deposits were plated onto mild steel followed by the rf magnetron sputtered chromium nitride thin film. Mechanical properties and tribological behavior of the duplex and single coating assemblies, including CrN, as-deposited EN and heat-treated EN on mild steel were examined. A significant increase of the surface hardness of the CrN on mild steel (CrN/MS) assembly was achieved by the addition of the EN interlayer. The strengthening of the CrN/MS coating system by the modification of the interlayer was evidenced through the indentation behavior analysis. It was also observed that the EN interlayer acted as a suitable underlying material beneath chromium nitride film to provide the required load-supporting ability for the CrN/MS coating composite during the dry pin-on-disc sliding process.