Zeolites are crystalline microporous aluminosilicates with high hydrothermal stability and strong solid acidity. However, pore blockage caused by coking, and reduced yields and selectivities caused by the slow diffusion rate of reactants and products in zeolite micropores (typically smaller than 1.4 nm) are problems that routinely arise in catalytic applications of zeolites. On the other hand, mesoporous materials with large uniform pore size of 2-50 nm are more suitable for the diffusion of large molecules. Then, this study attempted to synthesis an mesoporous aluminosilicate with zeolite building unit. LTA(Na-A type zeolite) in a HCl solution were used as a single-source of silicon and aluminum for the synthesis of mesoporous aluminosilicates via a template-assisted method with an amphiphilic triblock copolymer Pluronic F127 (EO106PO70EO106). Decreasing the concentration of HCl solution in dissolved LTA resulted in an increase in the aluminum content of the products. Pore size and pore wall thickness was increased with higher content of aluminum incorporated into the mesoporous framework. All samples have successfully possessed highly ordered mesoporous structure. The samples with Si/Al ratio of 12.6, which prepared at HCl concentration of 2.3 mol/L in dissolved LTA solution, possess BET surface area of 855 m2/g, pore size of 8.3 nm, and pore volume of 0.75 cm3/g. Aluminum atoms have been incorporated in a tetrahedrally and octahedrally coordinated position and remained stable even after calcination at 600 ◦C.