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Soft actuators are typically designed to be inherently stress‐free and stable. Relaxing such a design constraint allows exploration of harnessing mechanical prestress and elastic instability to achieve potential high‐performance soft robots. Here, the strategy of prestrain relaxation is leveraged to design pre‐curved soft actuators in 2D and 3D with tunable monostability and bistability that can be implemented for multifunctional soft robotics. By bonding stress‐free active layer with embedded pneumatic channels to a uniaxially or biaxially pre‐stretched elastomeric strip or disk, pre‐curved 2D beam‐like bending actuators and 3D doming actuators are generated after prestrain release, respectively. Such pre‐curved soft actuators exhibit tunable monostable and bistable behavior under actuation by simply manipulating the prestrain and the biased bilayer thickness ratio. Their implications in multifunctional soft robotics are demonstrated in achieving high performance in manipulation and locomotion, including energy‐efficient soft gripper to holding objects through prestress, fast‐speed larva‐like jumping soft crawler with average locomotion speed of 0.65 body‐length s−1 (51.4 mm s−1), and fast swimming bistable jellyfish‐like soft robot with an average speed of 53.3 mm s−1. [ABSTRACT FROM AUTHOR]