We report a visible light-responsive bilayer actuator driven by the photothermal properties of a unique molecular photoswitch: donor–acceptor Stenhouse adduct (DASA). We demonstrate a synthetic platform to chemically conjugate DASA to a load-bearing poly­(hexyl methacrylate) (PHMA) matrix via Diels–Alder click chemistry that enables access to stimuli-responsive materials on scale. By taking advantage of the negative photochromism and switching kinetics of DASA, we can tune the thermal expansion and actuation performance of DASA–PHMA under constant light intensity. This extends the capabilities of currently available responsive soft actuators for which mechanical response is determined exclusively by light intensity and enables the use of abundant broadband light sources to trigger tunable responses. We demonstrate actuation performance using a visible light-powered cantilever capable of lifting weight against gravity as well as a simple crawler. These results add a new strategy to the toolbox of tunable photothermal actuation by using the molecular photoswitch DASA.

We report the synthesis of diblock poly-amido-saccharides (PASs) by sequential addition of variably protected glucose and galactose monomers via living anionic ring-opening polymerization. Diblock polymers with varied polymer length, hydrophobic to hydrophilic ratio, and stereochemistry of hydrophilic component were synthesized, characterized by NMR, IR, and GPC. These amphiphilic polymers self-assemble in water to form nanoparticles as determined by DLS, SEM, and cryo-TEM. Amphiphilic polymers with glucose-PAS hydrophobic and galactose-PAS hydrophilic blocks and degree of polymerization of 100 (100-EtGlc1-OHGal3diblock PAS) form spherical nanostructures and are non-cytotoxic.