In this work, a supertough, self-healable, and extreme-environment-tolerable liquid metal (LM) composite organohydrogel was fabricated by dispersing LM particles (LMPs) with water-soluble starch (WS) and leveraging multilevel hydrogen-bonding interactions. Attributed to the cooperation of the strong dual-hydrogen bonds and weak monohydrogen bonds, the organohydrogel obtained an outstanding tensile strength of 2.0 ± 0.13 MPa and toughness of 16.0 ± 1.0 MJ m