With the morphological transformation of fluorescent self-assembled nanostructures, their functions can be varied simultaneously. However, little attention has been paid to the function variation in this process. Herein, we present aggregation-induced emission (AIE)-active self-assembled nanospheres to investigate the transformation-induced function variation by switching the energy dissipation pathway. The self-assembled nanospheres showed strong emission under neutral conditions, indicating that radiative decay dominates the energy dissipation. Under acidic conditions, the spheres transformed to vesicles and nanotubes, in which the excited energy was largely consumed by the intersystem crossing pathway and highly efficient reactive oxygen species (ROS) generation was afforded. In particular, this morphological transformation and function variation can smoothly proceed in acidic lysosomes, thus drastically boosting photodynamic cancer therapy.