Tough protein organohydrogels were fabricated by applying a solvent displacement-induced toughening (SDIT) strategy. With SDIT, traditionally weak and brittle protein hydrogels were altered to protein organohydrogels with remarkably high performance in anti-freezing, non-drying, topological healing, thermal plasticizing, mechanical toughness and stretchability. The SDIT opens a reliable and straightforward path to develop novel biomimetic materials and artificial devices from abandunt protein-based sources.