shows that surface oxides that form upon ambient exposure on superconducting metals such as Ta, Al, and Nb host two-level system (TLS) defects, which are a leading source of microwave loss and decoherence. While the surface oxides of Nb and Al have been extensively studied, Ta oxides remain less well understood. Using secondary ion mass spectrometry of alpha-Ta films deposited at 300 mm wafer scale, we show for the first time that hydroxyls accumulate in the Ta suboxide region above the underlying Ta. Angle-resolved X-ray photoelectron spectroscopy shows that the surface region is dominated by Ta2O5, with sub-stoichiometric TaOx present in between the Ta2O5 and underlying Ta. The thickness of the tantalum oxide is confirmed by transmission electron microscopy. We demonstrate that [OH] incorporation can be suppressed by replacing the native oxide with an oxide formed during chemical mechanical planarization of alpha-Ta films. Our findings support the hypothesis that TLS defects are non-uniform within the oxide thickness and suggest hydroxyls as a probable molecular origin of these loss channels. Furthermore, we show the feasibility of plasma nitridization as a method to decrease hydroxyl loading on alpha-Ta surfaces. The modulation of hydroxyl content through surface engineering of alpha-Ta can enable the fabrication of more robust, high-coherence superconducting quantum circuits by addressing a potential TLS source.