Predictable bending deformation, high cycle stability, and multimode complex motion have always been the goals pursued in the field of flexible robots. In this study, inspired by the delicate structure and humidity response characteristics of Selaginella lepidophylla, a new multilevel assisted assembly strategy was developed to construct MXene-CoFe2O4 (MXCFO) flexible actuators with different concentration gradients, to achieve predictable bending deformation and multi-stimulus cooperative control of the actuators, revealing the intrinsic link between the gradient change and the bending deformation ability of the actuator. The thickness of the actuator shows uniformity compared with the common layer-by-layer assembly strategy. And, the bionic gradient structured actuator shows high cycle stability, and it maintains excellent interlayer bonding after bending 100 times. The flexible robots designed based on the predictable bending deformation and the multi-stimulus cooperative response characteristics of the actuator initially realize conceptual models of humidity monitoring, climbing, grasping, cargo transportation, and drug delivery. The designed bionic gradient structure and unbound multi-stimulus cooperative control strategy may show great potential in the design and development of robots in the future.
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