▎ 摘　　要

Gaining spatially resolved control over the mechanical properties of materials in a remote, programmable, and fast-responding way is a great challenge toward the design of adaptive structural and functional materials. Reversible, temperature-sensitive systems, such as polymers equipped with supramolecular units, are a good model system to gain detailed information and target large-scale property changes by exploiting reversible crosslinking scenarios. Here, it is demonstrated that coassembled elastomers based on polyglycidols functionalized with complementary cyanuric acid and diaminotriazine hydrogen bonding couples can be remotely modulated in their mechanical properties by spatially confined laser irradiation after hybridization with small amounts of thermally reduced graphene oxide (TRGO). The TRGO provides an excellent photothermal effect, leads to light-adaptive steady-state temperatures, and allows local breakage/de-crosslinking of the hydrogen bonds. This enables fast self-healing and spatiotemporal modulation of mechanical properties, as demonstrated by digital image correlation. This study opens pathways toward light-fueled and light-adaptive graphene-based nanocomposites employing molecularly controlled thermal switches.