AbstractSoft robots have the potential to assist and complement human exploration of extreme and harsh environments (i.e., organic solvents). However, soft robots with stable performance in diverse organic solvents are not developed yet. In the current research, a non‐Euclidean‐plate under‐liquid soft robot inspired by jellyfish based on phototropic liquid crystal elastomers is fabricated via a 4D‐programmable strategy. Specifically, the robot employs a 3D‐printed non‐Euclidean‐plate, designed with Archimedean orientation, which undergoes autonomous deformation to release internal stress when immersed in organic solvents. With the assistance of near‐infrared light illumination, the organic solvent inside the robot vaporizes and generates propulsion in the form of bubble streams. The developed NEP‐Jelly‐inspired soft robot can swim with a high degree of freedom in various organic solvents, for example, N, N‐dimethylformamide, N, N‐dimethylacetamide, tetrahydrofuran, dichloromethane, and trichloromethane, which is not reported before. Besides bionic jellyfish, various aquatic invertebrate‐inspired soft robots can potentially be prepared via a similar 4D‐programmable strategy.