The channel walls of periodic mesoporous silica were modified with nitrogen-containing aromatic molecules through a metalorganic route, utilizing the lithiated aromatic core under mild reaction conditions and short reaction times. The functionalities grafted to the silica walls include primary and tertiary amines, as well as pyridine, pyrimidine and nitrobenzene. The new hybrid materials were characterized with X-ray diffraction, electron microscopy, thermogravimetry, nitrogen sorption, as well as Raman and UV-vis spectroscopies. The metalorganic modification of mesoporous molecular sieves with functional aromatics proves to be a fast, simple and economic method for the design of novel mesoporous inorganic - organic hybrid systems.