To develop efficient dual-function materials (DFMs) for capture and destruction of volatile organic compounds (VOCs), we prepared a series of composite materials comprising PtNi nanoparticles supported on ZrO2-promoted SiO2(PtNi/ZrO2-SiO2) via atomic layer deposition (ALD) method and investigated them for sequential adsorption and desorption/catalytic oxidation of benzene, as a model VOC compound. ZrO2was first deposited on a unimodal SiO2support, followed by deposition of Pt and Ni nanoparticles with varried amount. Dynamic adsorption experiments were conducted using a 500 ppmv-laden feed at 25 °C and 1 atm, followed by in situ catalytic oxidation at 200 °C. Among the DFMs investigated, 1Pt2Ni/ZrSi emerged as the material with overall in situ conversion of ∼96% due to its retaively high PtNi acid sites density compared with other DFMs. Kinetic analysis was conducted on 1Pt2Ni/ZrSi by investigating the effects of feed concentration, regenerative feed flow rate, and oxidation temperature on the benzene conversion in the sequential adsorption-oxidation process. The results of the kinetic analysis revealed that a complete oxidation can be attained over 1Pt2Ni/ZrSi and its performance can be improved upon decreasing adsorptive feed benzene concentration (maximum value of 99.7% at 125 ppmv) and regenerative feed flow rate (100% at 5 mL/min), and increasing oxidation temperature (100% at 200 °C). Overall, the obtained results highlighted the optimal operation conditions for sequential adsorption and oxidation of VOCs over ALD-based DFMs.