Dendrimers based on melamine have been covalently attached to silica gel with convergent and divergent approaches. These approaches yield different products. Each step of the synthesis can be monitored with Fourier transform infrared spectroscopy, thermal gravimetric analysis, and X-ray photoelectron spectroscopy. The organic molecules can be isolated by chemical etching the organosilica material with HF and then analyzed by mass spectrometry. The convergent approach, which relies on the solution-phase synthesis of the dendrimer before its attachment onto silica gel, produces materials that are similar to20% w/w organic regardless of the generation of the dendrimer used in the preparation of these composites and without apparent defects in the dendrimer structure. Materials prepared with the divergent approach show increasing percentages of organic material with each generation, but the dendrimers show structural defects including incomplete branching. In a survey of sequestration potential, materials obtained with the divergent approach removed more atrazine from solution than the more homogeneous materials obtained from the convergent approach. (C) 2004 Wiley Periodicals, Inc.