Nitration of 1,3,3-trimethyl-1-phenylindane (phenylindane) by nitric acid of different concentration over mesoporous aluminosilicates with the molar ratios SiO2 : Al2O3 = 20, 40, and 80 was studied. The effects of the SiO2 : Al2O3 and phenylindane : nitric acid ratios, the concentration of nitric acid, and temperature on the conversion of phenylindane and the yield of dinitrophenylindane were revealed. The aluminosilicate samples with a SiO2 : Al2O3 ratio of 20 are shown to have the highest activity. In the presence of these samples, the conversion of phenylindane reaches 100% with a selectivity of formation of 5and 6-nitro-1-(4´-nitrophenyl)1,3,3-trimethylindanes close to 80% (70% nitric acid, 100 °C).