The development of promising new high-performance materials, such as composite materials made of fibers in a polymeric resin (fiber-reinforced polymer, or FRP), has transformed the structural rehabilitation and upgrade industry for buildings and infrastructure. Conventional materials and construction techniques (e.g., strengthening with externally bonded steel plates, known as beton plaqués, or steel/concrete jackets) have been supplanted by innovative ones. The most important emerging techniques involve the use of externally bonded composites as a quick and effective option for repairing and upgrading existing structures. Several issues regarding FRP–substrate interaction, mainly related to brittle failure mechanisms due to fracture phenomena, remain the focus of a great deal of research. This paper presents an overview of debonding behavior and its predictive modelling in externally bonded FRP systems.