The adsorption of a range of molecular species (water, pyridine, and ammonia) is found to reversibly modulate the conductivity of hydrogen-terminated silicon-on-insulator (H-SOI) substrates. Simultaneous sheet-resistance and Hall-effect measurements on moderately doped (1015 cm−3) n- and p-type H-SOI samples mounted in a vacuum system are used to monitor the effect of gas exposure in the Torr range on the electrical-transport properties of these substrates. Reversible physisorption of “hole-trapping” species, such as pyridine (C5H5N) and ammonia (NH3) produces highly conductive minority-carrier channels (inversion) on p-type substrates, mimicking the action of a metallic gate in a field-effect transistor. The adsorption of these same molecules on n-type SOI induces strong electron-accumulation layers. Minority/majority channels are also formed upon controlled exposure to water vapor. These observations can be explained by a classical band-bending model, which considers the adsorbates as the source of a uniform surface charge ranging from +1011 to +1012q cm−2. These results demonstrate the utility of DC transport measurements of SOI platforms for studies of molecular adsorption and charge-transfer effects at semiconductor surfaces.