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A novel soft actuator is designed, fabricated, and optimized from liquid marbles encased via interfacial polymerization for added mechanical strength and robustness. They are encased in bimorph-type soft actuators where one side of the actuator has a dramatically different Young’s modulus than the other, leading to directional actuation which is successfully demonstrated in multistep walking soft robots. The soft actuators were also shown to successfully activate the mechanosensitive Piezo protein in a transfected human cell line, 293T. Overall, the liquid marble powered soft actuators described here represent a new soft actuation methodology and a novel tool for mechanobiological studies.