Coatings have become one of the most ubiquitous end applications for polymeric materials. Introducing self-repairing mechanisms into coatings is one way to ensure a high level of performance and an extended service life-time, with reduced energy and cost efforts with maintenance and repair. This chapter presents a revision of the self-healing approaches and mechanisms that have the potential to find applications in the broad and challenging smart coatings field. It discusses some of the systems/mechanisms, in light of main molecular interactions that can be used to introduce intrinsic healing mechanisms on polymeric coatings: (i) molecular chains inter-diffusion and segregation, (ii) reversible bonds, and (iii) noncovalent bonds. Many of the current functional polymeric coatings rely on their surface chemical groups for a special performance or functionalities, such as extreme water repellence, self-cleaning behavior (via superhydrophobic or superhydrophilic mechanisms), or anti-(bio)adhesion (i.e., low adherence of proteins and other biofoulants).