A combinatorial material adhesion study was used to optimize the composition of an adhesion promoting layer for a nanocrystalline diamond (NCD) coating on silicon. Three different adhesion promoting metals, namely W, Cr, and Ta, were selected to fabricate arrays of co-sputtered binary alloy films, with patches of seven different, distinct alloy compositions for each combination, and single element reference films on a single Si wafer (three wafers in total; W–Cr, Cr–Ta, Ta–W). Scratch testing was used to determine the critical failure load and practical work of adhesion for the NCD coatings as a function of adhesion layer chemistry. All tested samples eventually exhibit delamination of the NCD coating, with buckles radiating perpendicularly away from the scratch track. Application of any of the presented adhesion layers yields an increase of the critical failure load for delamination as compared to NCD on Si. While the influence of adhesion layers on the maximum buckle length is less pronounced, shorter buckles are obtained with pure W and Cr–Ta alloy layers. As a general rule, the addition of an adhesion layer showed a 75% improvement in the measured adhesion energies of the NCD films compared to the NCD coating without an adhesion layer, with specific alloys and compositions showing up to 125% increase in calculated practical work of adhesion.Read less <