Abstract This paper focuses on the frictional behavior of flexible diamond-like carbon (DLC) film-coated hydrogenated nitrile butadiene rubber. By making use of the substantial thermal mismatch between DLC film and rubber substrate, a dense network of cracks forms in the DLC films and contributes to flexibility. The influence of the size of DLC film microsegments on the frictional performance is studied. The effect of viscoelasticity of the rubber substrate on the frictional behavior of the DLC film-coated system is scrutinized by tribo-tests and theoretical analysis. The importance of adhesive and hysteresis contributions to friction is revealed, and an overarching model is presented.