A novel self-oscillating polymer was prepared by utilizing the Belousov-Zhabotinsky (BZ) reaction. In this study, a sulfonic acid group was newly introduced as a pH-control site into the copolymer of N-isopropylacrylamide, and the ruthenium complex was introduced as a catalyst site. By introducing the pH-control site, we succeed in causing the soluble-insoluble self-oscillation of the polymer solution under acid-free conditions in which only two BZ substrates, malonic acid and sodium bromate, were present as added agents. The self-oscillating behavior was remarkably influenced by the temperature and polymer concentration, which reflects the intermolecular aggregative capacity of the polymer chains in the reduced state to change the lower critical solution temperature. This achievement of self-oscillation of polymer chains under acid-free conditions may lead to their practical use as novel biomimetic materials under biological conditions.