Polymer nanodiscs, especially with stimuli‐responsive features, represent an unexplored frontier in the nanomaterial landscape. Such 2D nanomaterials are however considered highly promising for advanced biomedicine applications. Herein, we designed a coil‐rod copolymer architecture based on an amphiphilic, tadpole‐like bottlebrush copolymer, which can directly self‐assemble into core‐shell nanodiscs in an aqueous environment. As the bottlebrush side chains are made of amorphous, UV‐responsive poly (ethyl glyoxylate) (PEtG) chains, they can undergo rapid end‐to‐end self‐immolation upon light irradiation. This triggered nanodisc disassembly can be used to boost small molecule release from the nanodisc core which is further aided by a morphological change from discs to spheres.