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Shape-morphing hydrogels have drawn great attention due to their wide applications as soft actuators, while asymmetric responsive shape-morphing behavior upon encountering external stimuli is fundamental for the development of hydrogel actuators. Therefore, in this work, bilayer hydrogels were prepared and the shrinkage ratios (LA/LN) of the AAm/AAc layer to the NIPAM layer immersed in different metal ion solutions, leading to bending in different directions, were investigated. The difference in the shrinkage ratio was attributed to the synergistic effect of the osmolarity difference between the inside and outside of the hydrogels and the interaction difference between the ion and hydrogel polymer chains. Additionally, under thermal stimuli, the hydrogel actuator would bend toward the NIPAM layer due to the shrinkage of the hydrogel networks caused by the hydrophilic–hydrophobic phase transition of NIPAM blocks above the LCST. This indicates that metal ion and thermal-responsive shape-morphing hydrogel actuators with good mechanical properties could be used as metal ion or temperature-controllable switches or other smart devices.