Due to their excellent biocompatibility, outstanding mechanical properties, high strength-to-weight ratio, and good corrosion resistance, titanium (Ti) alloys are extensively used as implant materials in artificial joints. However, Ti alloys suffer from poor wear resistance, resulting in a considerably short lifetime. In this study, we demonstrate that the chemical self-assembly of novel two-dimensional (2D) diamond nanosheet coatings on Ti alloys combined with natural silk fibroin used as a novel lubricating fluid synergistically results in excellent friction and wear performance. Linear-reciprocating sliding tests verify that the coefficient of friction and the wear rate of the diamond nanosheet coating under silk fibroin lubrication are reduced by 54 and 98%, respectively, compared to those of the uncoated Ti alloy under water lubrication. The lubricating mechanism of the newly designed system was revealed by a detailed analysis of the involved microstructural and chemical changes. The outstanding tribological behavior was attributed to the establishment of artificial joint lubrication induced by the cross binding between the diamond nanosheets and silk fibroin. Additionally, excellent biocompatibility of the lubricating system was verified by cell viability, which altogether paves the way for the application of diamond coatings in artificial Ti joint implants.