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Iron and chromium modified aluminosilicate mesostructure adsorbents (Fe-MSU-S and Cr-MSU-S) were prepared in order to selectively remove nitrogen compounds from model fuel containing quinoline, carbazole, benzothiophene and dibenzothiophene. Characterization techniques such as scanning electron microscopy (SEM), low temperature N2 adsorption-desorption (BET) and fourier transform infrared spectroscopy (FT-IR) were employed for determining the optimum parameters during the adsorbent synthesis. Fe and Cr impregnation caused a negative effect on mesoporous structure, crystalline phase, and particle shape along with a positive impact on surface acidity which prevailed over negative ones and consequently led to improvement of S/N adsorption compared to MSU-S. The results demonstrated that iron enhanced the quinoline and carbazole uptake of MSU-S by 38.8% and 17.8%, respectively. The maximum adsorption capacities of Cr-MSU-S as compared to pristine MSU-S for quinoline and carbazole were improved by 22.4% and 11.76%, respectively. The adsorption mechanism may be attributed to the acid-base interaction.