In this work, we study the effects of treating nanostructured SnO2–SiO2 films derived by a sol-gel method with nitrogen and oxygen plasma. The structural and chemical properties of the films are closely investigated. To quantify surface site activity in the films following treatment, we employed a photocatalytic UV degradation test with brilliant green. Using X-ray photoelectron spectroscopy, it was found that treatment with oxygen plasma led to a high deviation in the stoichiometry of the SnO2 surface and even the appearance of a tin monoxide phase. These samples also exhibited a maximum photocatalytic activity. In contrast, treatment with nitrogen plasma did not lead to any noticeable changes in the material. However, increasing the power of the plasma source from 250 W to 500 W led to the appearance of an SnO fraction on the surface and a reduction in the photocatalytic activity. In general, all the types of plasma treatment tested led to amorphization in the SnO2–SiO2 samples.