Chemisorption of pyridine and atmospheric CO2 followed by means of visible Raman and DRIFT spectroscopy were employed to investigate the surface acidity and structure of as-prepared SrTiO3 (STO) samples synthesized using three different approaches, solid-state reaction, molten salt, and sol-precipitation–hydrothermal treatment. Samples prepared via solid-state reaction consisted of irregularly shaped polycrystalline grains with a BET surface area of ∼2 m2/g, whereas those obtained via molten salt synthesis and sol-precipitation–hydrothermal treatment were single-crystalline nanocubes with the {100} faces primarily exposed and BET surface areas of ∼10 and 20 m2/g, respectively. Pyridine and atmospheric CO2 chemisorption demonstrated that the differences in surface acidity between samples synthesized using different approaches are rather slight with a mixture of SrO-based and TiO-based terminations observed in all cases. In contrast, the typology of surface carbonate species arising from the reactive adsorp...