A new two-step synthesis of ZrO 2-MCM nanocomposites using the gel combustion technique was accomplished; the resulting material had a high-surface area and showed very high adsorption activity. The deposition of 2-5 nm ZrO 2 particles over MCM was achieved using gel combustion technique with glycine as a fuel, and the formation of nanocomposites was confirmed using transmission electron microscopy. The composites were also characterized by XRD, SEM, FTIR and N 2 adsorption-desorption analysis. The nanocomposites were tested for the adsorption of cationic dyes. High rates of adsorption and large dye uptake were observed over the nanocomposites. The rate of adsorption over the nanocomposites was higher than that observed for physical ZrO 2-MCM mixtures and commercial activated carbon. The nanocomposite with 10 wt % ZrO 2 showed the highest rate of adsorption owing to the synergistic effects of ZrO 2 surface groups, smaller particle size, fine dispersion and high-surface area of the composite. © 2012 American Institute of Chemical Engineers (AIChE).