Metal-organic frameworks (MOFs) are witnessing rapid development in the adsorption removal of volatile organic compounds (VOCs) from polluted air due to their remarkable adsorption capacity. However, their intrinsic poor thermal conductivities often make their regeneration processes suffer from high energy consumption. Herein, a novel photodynamic NH2-UiO-66@PPy adsorbent was constructed by in-situ growth of NH2-UiO-66 particles onto hollow PPy nanotubes via a facile solvothermal method. This adsorbent was able to extend the light response range of NH2-UiO-66 from UV–vis to near-infrared region. Benefitting from the superior photothermal conversion ability of PPy and well contact interface between PPy nanotube and its surface-loaded NH2-UiO-66 particles, higher surface temperature of PPy nanotubes would be obtained upon exposure to UV–vis-NIR light and further transferred to its surrounding MOF nanoparticles. Eventually, the surface temperature of the optimal NH2-UiO-66@PPy-2 adsorbent can be as high as 245 °C, and almost 100% of the adsorbed ethyl acetate was able to be released within 30 min of UV–vis-NIR irradiation. Distinct from the conventional heating whole adsorbent bed, this photothermal desorption strategy would significantly reduce the heat-transfer among adsorbent particles and become less dependent on the heat-transfer rate, thus efficiently alleviating the intrinsic thermal conductivity shortcoming of MOF.