Recent studies have shown that dynamic nuclear polarization (DNP) can be used to detect 17O solid-state NMR spectra of naturally abundant samples within a reasonable experimental time. Observations using indirect DNP, which relies on 1H mediation in transferring electron hyperpolarization to 17O, are currently limited mostly to hydroxyls. Direct DNP schemes can hyperpolarize non-protonated oxygen near the radicals; however, they generally offer much lower signal enhancements. In this study, we demonstrate the detection of signals from non-protonated 17O in materials containing silicon. The sensitivity boost that made the experiment possible originates from three sources: indirect DNP excitation of 29Si via protons, indirect detection of 17O through 29Si nuclei using two-dimensional 29Si{17O} D-HMQC, and Carr-Purcell-Meiboom-Gill refocusing of 29Si magnetization during acquisition. This 29Si-detected scheme enabled, for the first time, 2D 17O−29Si heteronuclear correlation spectroscopy in mesoporous silica and silica-alumina surfaces at natural abundance. In contrast to the silanols showing motion-averaged 17O signals, the framework oxygens exhibit unperturbed powder patterns as unambiguous fingerprints of surface sites. Along with hydroxyl oxygens, detection of these moieties will help in gaining more atomistic-scale insights into surface chemistry.