Large　amounts　of　anthropogenic　VOCs　emissions　give　rise　to　photochemical　smog　and　ground-level　ozone.　Currently,　catalytic　oxidation　for　VOCs　elimination　still　requires　energy-intensive　high　temperatures.　Lightdriven　photo-thermocatalysis　oxidation　of　VOCs　holds　great　promise　to　substantially　reduce　energy　consumption　for　sustainable　development　in　comparison　with　conventional　thermal-based　catalytic　oxidation.　Herein,　CeO2/LaMnO3　composite,　featuring　the　broad　light　wavelength　absorption　(800　similar　to　1800　nm),　can　be　used　as　a　highly　active　photo-thermal　responsive　catalyst　on　VOCs　decomposition　under　IR　irradiation.　The　maximum　photothermal　conversion　efficiency　is　able　to　reach　15.2%　with　a　significant　toluene　conversion　of　89%　and　CO2　yield　of　87%　under　IR　irradiation　intensity　of　280　mW/cm(2),　together　with　excellent　stability　of　nearly　30　h.　Comparative　characterizations　reveal　that　such　photo-thermal　catalytic　activity　enhancement　is　predominantly　attributed　to　the　synergistic　effects　of　ultrabroadband　strong　light　absorption,　efficient　light-to-heat　conversion,　good　low　temperature　reducibility　and　high　lattice　oxygen　mobility,　originating　from　an　intense　interaction　of　LaMnO3　with　CeO2.　Toluene　oxidation　reaction　on　CeO2/LaMnO3　catalyst　proceeds　via　a　Mars-van　Krevelen　mechanism　as　evidenced　by　in　situ　diffuse　reflectance　infrared　Fourier　transform　spectroscopy.