Controlled release systems have gained considerable attention owing to their potential to deliver molecules, including ions and drugs, in a customized manner. We present a light‐induced ion‐transfer platform consisting of a dispersion of nanoparticles (NPs, ~300 nm) with the conductive polymer poly(3‐octylthiophene‐2,5‐diyl) (POT) in the core and a potassium (K+)‐selective membrane in the shell. Owing to the photoactive nature of POT, each NP can be used for a dual purpose: as a host for positively charged species and as an actuator to trigger the subsequent release. POT0 and doped POT+ coexist in the core, allowing K+ encapsulation in the shell. As POT0 is photo‐oxidized to POT+, K+ is released to the (aqueous) dispersion phase to preserve the neutrality. This process is reversible and can be assessed using the native fluorescence of POT0 and via potentiometric measurements. The NP structure and its mechanism of action were thoroughly studied with a series of control experiments and complementary techniques. Understanding the NP and its surrounding interactions will pave the way for other nanostructured systems, facilitating sophisticated applications. The delivery of ionic drugs and interference/pollutant catching for advanced sensing/restoration will be considered in future research.