Volatile organic compounds (VOCs) are prevalent soil contaminants. During the ex situ soil remediation process, VOCs may overflow from the soil and cause gas to diffuse into the atmosphere. Moreover, some VOCs, such as trichloromethane, are categorized by the EPA as emerging contaminants, imparting toxicity to organs, and the endocrine and immune systems, and posing a huge threat to human health and the environment. To reduce VOCs’ emissions from contaminated soil, aqueous foam suppression is a prospective method that provides a durable mass transfer barrier for VOCs, and it has been widely used in odor control. Based on an aqueous foam substrate, in order to enhance the foam’s stability and efficiency of suppression, SiO2–TiO2-modified nanoparticles have been used as stabilizing agents to improve the mechanical strength of liquid film. The nanoparticles are endowed with the ability to photocatalyze after the introduction of titanium dioxide. From SEM imaging, IR, and a series of morphological characterization experiments, the dispersibility of the SiO2–TiO2-modified nanoparticles was significantly improved under the polar solvent, which, in turn, increased the foam duration. The foam dynamic analysis experiments showed that the foam liquid half-life was increased by 4.08 h, and the volume half-life was increased by 4.44 h after adding the novel synthesized nanoparticles to the bulk foam substrate. From the foam VOC suppression test, foam with modified nanoparticles was more efficient in terms of VOCs’ suppression, in contrast with its nanoparticle-free counterparts, due to the longer retention time. Moreover, in a bench-scale experiment, the SiO2–TiO2 nanoparticles foam worked against dichloroethane, n–hexane, and toluene for almost 12 h, with a 90% suppression rate, under UV irradiation, which was 2~6 h longer than that of UV-free SiO2–TiO2 nanoparticles, the KH–570-modified nanosilica foam, and the nanoparticle-free bulk foam. XPS and XRD results indicate that in SiO2–TiO2 nanoparticles, the proportion of titanium valence was changed, providing more oxygen vacancies compared to raw titanium dioxides.