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Volatile organic compounds (VOCs) originating from diverse sources with complex compositions pose threats to both environmental safety and human health. Photocatalytic treatment of VOCs has garnered attention due to its high efficacy at room temperature. However, the intricate photochemical reaction generates ozone (O 3 ), causing secondary pollution. Herein, our work developed a novel "synergistic effect" system for photocatalytic co-treatment of VOCs and O 3 secondary pollution. Under the optimized reactor conditions simulated with computational fluid dynamics (CFD), MgO-loaded g-C 3 N 4 composites (MgO/g-C 3 N 4 ) were synthesized as efficient catalysts for the photocatalytic synergistic treatment process. Density functional theory (DFT) calculations, characterization, and electron paramagnetic resonance (EPR) tests revealed that the addition of MgO reduced the band gap of g-C 3 N 4 , and increased O 3 molecule adsorption in the composites, efficiently harnessing the synergistic effect of O 3 to generate a significant quantity of reactive oxygen radicals, thereby facilitating the removal of VOCs and O 3 . This study provides new insights for simultaneous elimination of VOCs and O 3 secondary pollution by a photocatalytic process., Competing Interests: There are no conflicts of interest to declare., (This journal is © The Royal Society of Chemistry.)