With the flourishing of mussel-inspired chemistry, the fast-growing development for environmentally friendly materials, and the need for inexpensive and biocompatible analogues to PDA in gel design, TA has led to its gradual emergence as a research focus due to its remarkable biocompatible, renewable, sustainable and particular physicochemical properties. As a natural building block, TA can be used as a substrate or crosslinker, ensuring versatile functional polymeric networks for various applications. In this review, the design of TA-based gels is summarized in detail (i.e., different interactions such as: metal coordination, electrostatic, hydrophobic, host–guest, cation-π and π-π stacking interactions, hydrogen bonding and various reactions including: phenol–amine Michael and Schiff base, phenol–thiol Michael addition, phenol–epoxy ring opening reaction, etc.). Subsequently, TA-based gels with a variety of functionalities, including mechanical, adhesion, conductive, self-healing, UV-shielding, anti-swelling, anti-freezing, shape memory, antioxidant, antibacterial, anti-inflammatory and responsive properties are introduced in detail. Then, a summary of recent developments in the use of TA-based gels is provided, including bioelectronics, biomedicine, energy, packaging, water treatment and other fields. Finally, the difficulties that TA-based gels are currently facing are outlined, and an original yet realistic viewpoint is provided in an effort to spur future development.