Highly dispersed and stabilized aluminosilicate nanoparticles were hydrothermally grown onto the surface of macroporous carbon with the aid of polyelectrolyte multilayer structure. The formation of the anchored aluminosilicate particles was followed by SEM and Al-27 solid-state NMR. The acidity of the carbon-supported aluminosilicate nanoparticles was evaluated by ammonia-TPD and n-hexane cracking, which exhibited activation energy of 12 kcal mole(-1). Impregnation of the carbon-supported aluminosilicate nanoparticles with aqueous solution of molybdenum citrate complex formed at pH 1.5 produced a supported MoS2 catalysts that exhibited HDS activity for 4,6-DMDBT similar to 3.5 times higher than its aluminosilicate-free analogue. The higher activity of the catalysts is attributed to a great extent to its enhanced hydrogenation ability with no significant contribution to other reactions. (C) 2009 Elsevier B.V. All rights reserved.