A bionic smart actuator that can imitate types of biological motions plays a vital role in intelligent systems, which therefore becomes one of the hottest development directions in recent years and has attracted more and more attention from researchers. In this study, a kind of near-infrared (NIR) light-responsive shape memory polyurethane SMPU-PB is developed by doping the citric acid-modified Prussian blue nanoparticles. Based on it, a bionic “athlete” has performed repeatable photomechanical jumping behavior to cross obstacles under 808 nm NIR light irradiation. Furthermore, through the integration of SMPU-PB with pre-strained UV-responsive polyurethane film, a hybrid wavelength-selective responsive structure capable of reversible, programmable, and controllable motions is produced. By using the two-way light-driven shape memory composite, the bionic actuator is able to complete a series of tasks including accurate bending and mechanical gripping.