Phenolic-compound-based functional coatings that allow for flexible modulation of chemical and surface properties have found widespread uses in a diverse range of biomedical applications from antibiofouling and antioxidation to bioimaging, therapeutics, and controlled drug delivery. It is imperative to understand the formation mechanism of phenolic coatings to fully meet the needs of their emerging applications in controlling the surface properties of biomaterials and medical devices. In this Perspective, we highlight the versatile chemical and self-assembly approaches to generate phenolic coatings with tailored surface properties and reactivities and also discuss how the surface properties and chemical reactivities impart functional materials for translational research.