This work reports on a novel ship-in-a-bottle strategy to fabricate DSCs with well-defined microstructure. The resulting DSCs exhibited outstanding performance toward catalytic ozonation of CH₃SH owing to the Fe 3d orbital coupling, which is of immediate interest to the DSCs synthesis but also to the reaction mechanism investigation of catalytic ozonation. Notably, the applicability of electron paramagnetic resonance (EPR) spectroscopy approach for determining ROS on the catalyst surface during ozonation processes, as well as the theoretical underpinnings for the transformation of surface oxygen species to ROS, warrants further in-depth investigation. Additionally, the use of DSCs for catalytic ozonation of a broader spectrum of VOC pollutants, beyond the specific case of CH₃SH oxidation, requires comprehensive evaluation.