Nitrous acid (HONO) is a household pollutant exhibiting adverse health effects and a major source of indoor OH radicals under a variety of lighting conditions. The present study focuses on gas-phase HONO and condensed-phase nitrite and nitrate formation on indoor surface thin films following heterogeneous hydrolysis of NO2, in the presence and absence of light, and nitrate (NO3-) photochemistry. These thin films are composed of common building materials including zeolite, kaolinite, painted walls, and cement. Gas-phase HONO is measured using an incoherent broadband cavity-enhanced ultraviolet absorption spectrometer (IBBCEAS), whereby condensed-phase products, adsorbed nitrite and nitrate, are quantified using ion chromatography. All of the surface materials used in this study can store nitrogen oxides as nitrate, but only thin films of zeolite and cement can act as condensed-phase nitrite reservoirs. For both the photo-enhanced heterogeneous hydrolysis of NO2 and nitrate photochemistry, the amount of HONO produced depends on the material surface. For zeolite and cement, little HONO is produced, whereas HONO is the major product from kaolinite and painted wall surfaces. An important result of this study is that surface interactions of adsorbed nitrite are key to HONO formation, and the stronger the interaction of nitrite with the surface, the less gas-phase HONO produced.