Physico-chemical properties of biointerfaces considerably determine the efficacy, biocompatibility, safety and durability of medical devices. For example, biomaterials-associated infections have been a major problem in modern medicine. Nowadays, there is no effective approach to defeat the infections, except for sterilization and uses of a plenty of antibiotics, which however contributes to the development of antibiotic resistant bacteria. The other surface-associated problems, such as thrombosis, foreign-body reaction, formation of protein corona on nanomaterials, and so on, remain troublesome. The state-of-the-art technologies for surface modification exhibit cumbersome procedure, instability, high-cost and lack of versatility. In this proposal, we aim to develop innovative bio-inspired “catecholic surface chemistries”. We will conjugate bio-inert moieties, i.e. zwitterionic groups, and bio-active moieties, i.e. biotin or folic acid, onto catecholic molecules to afford self-assembling bio-functional surface modifiers. Catecholic assemblies will effective form thin films to control interfacial properties and adsorption behaviors. The study is inspired from dopamine, which has been reported to substrate-independently adhere on surfaces. Its amine group will be converted to a variety of bio-functional moieties to construct a set of assemblies for surface engineering. Our preliminary results indicated that the zwitterionic dopamine enables to form thin films via a pH transition approach to resist non-specific adsorption of proteins, cells and bacteria. The fields of the research will cover from materials synthesis, physico-chemical fundamentals of catecholic attachment mechanism, and antimicrobial and biosensing applications. The intact contour of “catecholic surface chemistries” will be developed for their great scientific potentials and a wide spectrum of applications.Self-assembling materials have been greatly influential to surface science. The proposal will be devoted to bio-inspired “catecholic surface chemistries”. Studies from different angles will boost the advances in surface and biomaterials sciences. Last but not least, the outputs of the research will generally affect the establishment of biomedical industries and development of high-level talents.