A novel strategy to fabricate bilayer hydrogel actuators based on the asymmetric distribution of crystalline regions across the bilayer structures was proposed. By employing PVA polymer chains into an alkali solvent-derived chitosan hydrogel matrix, chitosan/PVA hybrid bilayer hydrogels with both excellent responsive bending and mechanical properties were obtained as pH-controlled manipulators. In the design, the chitosan/PVA hydrogels upon treatment with freeze-thawing cycles were taken as the first monolayer, where excessive crystalline regions appeared. The original chitosan/PVA hydrogel as the second monolayer was then integrated into one bilayer device through the chemical-crosslinking of epichlorohydrin at the interface. The results showed that the resultant chitosan/PVA bilayer hydrogel actuator with a weight ratio of 3 : 1 displayed better sensitivity upon exposure to stimuli. The actuation behaviors are strongly dependent on experimental parameters such as the pH, PVA content and the chemical-crosslinking density. It is proposed that the driving force originates from the asymmetric distribution of crystalline regions, thus resulting in differential swelling ratios between the monolayers. In addition, programmable 3D shape transformations were achieved by using the bilayer hydrogel with designed 2D geometric patterns, and the tailored gripper-like hydrogel actuator can successfully capture and transport the cargo. Moreover, this actuation behavior can be erased and re-written on demand under certain conditions. Taking advantage of this universal strategy, more attractive actuators derived from synthetic or natural polymers in combination with PVA are highly expected, which can be used as smart soft robots in various fields such as manipulators, grippers, and cantilever sensors.