A strategy of de novo peptides for customizing supramolecular self-assembly coating with desired biological functionalities

•A facile and efficient strategy for engineering the implant surface was developed.•The implant surface can be endowed with customized biological functionalities.•This strategy was free toxic agents, mild condition, simplicity and universality.•Deposition of peptide improved the inferior modulus and stability of original coating.•This strategy exhibits enormous potentials in various biomedical fields. The interfacial property of implant is of paramount importance in determining the eventual therapeutic outcomes. However, the mutative shapes and substrates of biomedical materials present significant challenges in engineering the implant surface to meet the requirement of complicated in vivo biological events. Herein, a facile and efficient strategy based on supramolecular self-assembly was developed, in which the de novo designed peptide (hexalysine, K6) was linked with bio-functional units (short or long peptides, and the synthetic polymer) and deposited onto metal-polyphenol networks (MPNs) coating, to endow the interface with desired biological functionalities, independent on shapes and materials of implant. The coating thickness, mechanism, kinetics, binding force and mode between K6 and polyphenol were thoroughly investigated by various techniques (AFM, SEM, XPS, ellipsometry, UV–vis). We found that K6 was able to penetrate through the MPNs, thereby significantly enhancing the poor modulus and poor stability of original MPNs. It is of significant importance to note that the bio-functionalities of linked units could be exploited to enhance cellular adhesion, osteogenesis, antibacterial and antifouling properties of the implants. The strategy capitalised on the free toxic agents, mild condition, simplicity and universality of preparation, enabling the customisation of biomedical implants with desired biological functionalities, which exhibited enormous potential in various biomedical fields.