MXene has been widely used in hydrogels due to its high electrical conductivity and surface tunability. However, its self-stacking behavior hinders its further utilization. To address that, we proposed a nanoengineering strategy that used sulfonated polyurethane nanoparticles (PU) to modify MXene, aiming to improve its dispersibility in the hydrogel precursor solution via the hydrogen bonding interactions between the sulfonic acid groups of PU and the oxygen-containing groups of MXene, which not only avoid the self-stacking of MXene but also endow the prepared hydrogel with ultrathinness of 32 μm, great stretchability of 1834%, high toughness of 385.6 KJ/m 3 as well as great puncture resistance, whose puncture displacement reached 85 mm at a thickness of 300 μm. Moreover, the hydrogel was also assembled as a strain sensor to monitor the human motions in real-time and recognize different hand gestures for human-machine interfaces. Furthermore, the hydrogel was capable of working as electrodes to assemble the trioelectric nanogenerators to power small devices for continuous energy supply. Overall, the developed ultrathin hydrogel fabricated via the nanoengineered MXene exhibited great potential in wearable electronics for flexible sensing, human-computer interaction, and self-powered devices.