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In this paper, we report a microcrack toughening mechanism for enhancing the adhesion of diamondcoating. The oriented microcracks were formed within the TiC interlayer to dissipate strain energy and accommodate deformation via the crack opening-closing mechanism, thus enhancing the coating/substrate interfacial toughness. The delamination of diamondcoating was effectively prevented when the parallel microcracks were confined within the interlayer and arrested at interfaces of coating/interlayer/substrate. Density functional theory calculations revealed that the highly anisotropicfracture strength of the TiC phase energetically favors crack initiation and propagation along (100) planes only, which are 54.7° away from the interface. These microcracks are constrained inside the interlayer by the two strong interfaces in the substrate/interlayer/coating system. The new microcrack toughening mechanism with these combined features has a wide application to enhance the adhesion of thin-film coatings.