A new facile synthesis of ordered mesoporous aluminosilicates has been developed and applied for the efficient catalytic synthesis of N-benzyl secondary amines under ligand and basefree conditions. The MAS(38) catalyst with a well-ordered mesoporous structure and strong acidic sites was used for acid-catalyzed organic transformations and its operational simplicity and ease of its isolation procedure make it an attractive alternative to current methodologies. N-alkyl secondary amine derivatives linked to herbicides and pharmaceuticals have been demonstrated as numerous biologically active compounds for drug discovery.[1] N-benzyl secondary amines, in particular, have attracted considerable attention from both biological and organic chemists. This is because they appear as carboxamide derivatives, which are the most prevalent structural moieties in medicinal chemistry.[2] However, despite widespread interest, the most common strategies for the production of secondary amines such as electrophilic alkylation, reductive alkylation, and amination of aryl halides, often exhibit limitations such as low selectivity toward desired secondary amines, harsh reaction conditions, and stoichiometric amounts of wasteful salts. [3,4] In addition, various expensive [Ru 3 (CO) 7 ] cluster, [Ir(COD)Cl] dimer, rhodium, and platinum transition metal complexes have been used as homogeneous catalysts for synthesizing secondary amines in the presence of base additives, which retard the commercialization of the process because of high cost and environmental concerns. [5][6][7] The use of heterogeneous catalysts [8][9][10][11][12] offers several advantages over homogeneous catalysts, including ease of separating reactants, minimal trace metal in the products, ease of handling, process control, and reusability of catalysts. These advantages can thus improve reaction processes. Therefore, developing an environmentally friendly and recyclable heterogeneous catalytic system for synthesizing secondary amines is of considerable interest. Heterogeneous catalysts such as Fe/ amino acids, Fe 3 O 4 , and Fe 3 O 4 /tBuO À have been used for the synthesis of secondary amines, [12,13] however, these systems suffer from complicated synthesis procedures and low activity compared with precious metal complexes.In recent years, mesoporous materials have demonstrated their potential in solar cells, fuel cells, and drug delivery systems. [14][15][16][17][18][19][20][21] In addition, mesoporous materials have been increasingly applied as heterogeneous catalysts in various organic transformations because of their unique structural and textural properties such as controllable pore size, uniform poresize distribution, high thermal stability, and ultrahigh specific surface area. [22,23] Among various heterogeneous catalysts, aluminosilicates have been considered useful solid catalysts because of their usage as effective catalysts in aldol, FriedelCrafts, and Diels-Alder reactions. [24,25] However, based on our knowledge, no studies have synthesized secondary amin...