The advance of microelectronics requires the micropower of microsupercapacitors(MSCs) to possess wide temperature-and damage-tolerance beyond high areal energy density.The properties of electrolyte are crucial for MSCs to meet the above requirements.Here,an organohydrogel electrolyte,featured with high salt tolerance,ultralow freezing point,and strong self-healing ability,is experimentally realized via modulating its inner dynamic bonds.Spectroscopic and theoretical analysis reveal that dimethyl sulfoxide has the ability to reconstruct Li+solvation structure,and interact with free water and polyvinyl alcohol chains via forming hydrogen bonds.The organohydrogel electrolyte is employed to build MSCs,which show a boosted energy density,promising wide temperature range-and damage-tolerant ability.These attractive features make the designed organohydrogel electrolyte have great potential to advance MSCs.