Material loss and plastic deformation induced by frictional interactions at moving mechanical interfaces continue to be major issues responsible for efficiency and performance degradation of systems. Establishment of fully elastic interactions in the contact region without compromising the structural rigidity and integrity of materials represents a promising solution. In this study, we report on improving the elasticity, damping properties, ductility and wear resistance of diamond-like carbon (DLC) coatings through introducing an immobilized C60 cluster layer. The C60 clusters were immobilized using cysteamine (HS(CH2)2NH2) self-assembled monolayers (SAMs) attached to a pre-sputtered Au layer. A Ni adhesive layer was deposited onto plasma cleaned Si (100) substrates prior to Au, SAM-C60, and DLC deposition. Precise dynamic ultra nano-indentation tests indicated a drastic improvement in elasticity and damping capacity of the C60-DLC hybrid (Ni-Au-SAM/C60-DLC) multilayer coating compared to those of the C60-free (Ni-Au-DLC) multilayer. The behavior of the coatings under reciprocating contact conditions was evaluated. Quantification of the resistance of the coatings against wear and permanent deformation revealed a significant improvement in the wear rate from ∼3.38 × 10-8 to ∼5.14 × 10-10 mm3 N-1 mm-1 upon incorporation of the immobilized C60 clusters. The corresponding mechanisms were assessed through experiments and finite element (FE) simulations.