This work represents the first precedent for the one-pot synthesis of ethanolamine-modified mesoporous silica. The resultant material was characterized by scanning electron microscopy, transmission electron microscopy, infrared spectroscopy, X-ray diffraction, and BET/BJH surface area/porosity measurements. The successful incorporation of ethanolamine moieties in the structure of mesoporous silica was confirmed by its subsequent reaction with phenyl isocyanate. The observed morphology of this surface-functionalized mesoporous silica is significantly different from that of postmodified SBA-15 and also features a greater porosity.