Fire-retardant coatings represent a universal cost-effective approach to providing fire protection for various substrates without compromising substrates’ bulk properties. However, it has been attractive yet highly challenging to create waterborne polymeric fire-retardant coatings combining high-efficiency, generally strong adhesion, and self-repairability due to a lack of rational design principles. Inspired by mussel's unique adhesive, self-healing, and char-forming mechanisms, herein, a “group synergy” design strategy is proposed to realize the combination of self-healing, strong adhesion, and high efficiency in a fully polymeric fire-retardant coating via multiple synergies between catechol, phosphonic, and hydroxyethyl groups. As-created fire-retardant coating exhibits a rapid room-temperature self-healing ability and strong adhesion to (non)polar substrates due to multiple dynamic non-covalent interactions enabled by these groups. Because these functional groups enable the formation of a robust structurally intact yet slightly expanded char layer upon exposure to flame, a 200 µm-thick such coating can make extremely flammable polystyrene foam very difficult to ignite and self-extinguishing, which far outperforms previous strategies. Moreover, this coating can provide universal exceptional fire protection for a variety of substrates from polymer foams, and timber, to fabric and steel. This work presents a promising material design principle to create next-generation sustainable high-performance fire-retardant coatings for general fire protection.