With their unique properties of self-healing and viscoelasticity, physically crosslinked supramolecular hydrogels are promising materials for soft robotics, wearable electronics and biomedical applications. However, the weak mechanical properties of supramolecular hydrogels, especially those prepared with natural polymers, limit their wide-spread application, and swelling is one of the key factors that contributes to the weakening of hydrogels. Herein, we utilize a simple one-pot solvent exchange method to prepare non-swellable, thermoplastic and tough supramolecular gelatin hydrogels based on two synergistic physical crosslinkings, namely, the self-assembled tri-helix structure of gelatin and the hydrophobic aggregation of gelatin-grafted and free hydrophobic motifs. The obtained hydrogels possess a stable water content above 70% with extended incubation in water. These hydrogels are highly malleable upon heating but are extremely stretchable and tough after cooling to room temperature. Furthermore, the supramolecular gelatin hydrogels exhibit robust adhesion to various material surfaces and minimal cytotoxicity. NPG Asia Materials (2018) 10, e455; doi:10.1038/am.2017.208; published online 5 January 2018 INTRODUCTION Hydrogels, due to their high water content and tunable physical and biological properties, are extensively used in soft robotics, wearable electronics and biomedical applications. 1-6 Supramolecular hydrogels, which are solely stabilized by physical crosslinkings, such as host-guest interactions, electrostatic attraction and hydrophobic aggregation, have recently received increasing attention due to their unique properties, including self-healing, energy dissipation and viscoelasticity. 7-13 However, the poor mechanical performance of supramolecular hydrogels, especially hydrogels prepared with natural polymers, which possess superior biocompatibility and bioactivity, remain a major hurdle to the wide-spread application of these hydrogels. To improve the mechanical properties of chemically crosslinked hydrogels, researchers have developed ingenious strategies, including nanocomposite hydrogels, double-network hydrogels, hybrid crosslinking hydrogels and tetra-polyethylene glycol hydrogels. [14][15][16][17][18][19][20][21][22] Recently, increasing research attention has been dedicated to enhancing the mechanical performance of physically crosslinked supramolecular hydrogels. One recent study demonstrated very tough physical hydrogels composed of polyampholytes. 23 Another study showed that pre-assembled host