Use of a given physiological stimulus to delicately deform polymer assemblies is a challenging topic. Here we develop synthetic block copolymers to construct a series of CO2-sensitive self-assembled nanostructures that can simulate controllable deformations of the organelles in different ways. By controlling the CO2 stimulation levels, one can modulate the size, shape, and morphology of the polymer aggregates, which is conducive to understanding the stimuli-triggered dynamic reshaping process of polymer assemblies in aqueous solution.