Supramolecular materials based on noncovalent bonds have attracted considerable attention in several fields due to their special characteristics such as self-healing, shape memory, and stimuli-responsive properties among others. [1][2][3][4][5][6][7][8][9][10] Indeed, multiple hydrogen bonding are ideal reversible noncovalent interactions for preparing supramolecular networks combining high strength and excellent reversibility. [11][12][13][14][15][16][17][18][19][20][21] Supramolecular Thermoresponsive Hydrogels Supramolecular hydrogels have promising applications in a wide variety of fields including 3D bioprinting, sensors and actuators, biomedicine, and controlled drug delivery. This communication reports the facile reversible thermotriggered formation of novel pH-responsive supramolecular hydrogels based on poly(vinyl alcohol) (PVA) bonded via dynamic H-bridge with small phenolic biomolecules. PVA and phenolic compounds form a clear solution when they are physically mixed in water at high temperature, but a fast gelation is produced at room temperature through multiple strong H-bonding interactions. The structure and type of functional groups of different phenolic molecules allow preparing hydrogels with tailor-made viscoelastic properties, controlled low phase transition temperature, and pH-dependent swelling behavior. This combination makes these supramolecular networks very interesting candidates to be used in 3D bioprinting and topical drug delivery of thermolabile biomolecules.