Bioinspired Hydroxyapatite Coating Infiltrated with a Graphene Oxide Hybrid Supramolecular Hydrogel Orchestrates Antibacterial and Self-Lubricating Performance

Hydroxyapatite (HA) bioceramic coating has been extensively applied for the modification of metallic implants to improve their biocompatibility and service life after implantation. Unfortunately, HA coating often suffers from high friction, severe wear, and bacterial invasion, which restrict its application in artificial joints. According to a bioinspired soft/hard combination strategy, a novel HA composite coating that is infiltrated with a vancomycin-loaded graphene oxide (GO) hybrid supramolecular hydrogel is developed via vacuum infiltration and a subsequent host–guest interaction-induced self-assembly process. The holes of textured HA ceramic coating act just like a “magic pocket”, offering a stable container to form and store GO hybrid hydrogels and even to recycle wear debris as well. The drug-loaded hybrid hydrogels stored in textured HA coating possess a unique shear force and/or frictional heat triggered gel–sol transition and sustained drug release behavior, acting like the extrusion of synovial fluid during articular cartilage movement, leading to a remarkable self-lubrication, anti-wear performance, and promising antibacterial property against Staphylococcus aureus. The friction coefficient and wear rate of composite coating reduced by nearly five times and three orders of magnitude compared with textured HA coating, respectively, which benefited from the synergistic lubricate effect of cyclodextrin-based pseudopolyrotaxane supramolecular hydrogel and GO lubricants.