Hydrogel-based shape-adjustable films were successfully fabricated via grafting poly(N-isopropylacrylamide) (PNIPAM) onto one side of polyimide (PI) films. The prepared PI-g-PNIPAM films exhibited rapid, reversible, and repeatable bending/unbending property by heating to near-human-body temperature (37 °C) or cooling to 25 °C. The excellent property of PI-g-PNIPAM films resulted from a lower critical solution temperature (LCST) of PNIPAM at about 32 °C. Varying the thickness of PNIPAM hydrogel layer regulated the thermo-responsive shape bending degree and response speed of PI-g-PNIPAM films. The thermo-induced shrinkage of hydrogel layers can tune the curvature of PI films, which have potential applications in the field of wearable and implantable devices.