Mesoporous aluminosilicates Al-SBA-15 with large pore sizes and suitable acid properties are promising substitutes to zeolites for catalytic cracking of bulky hydrocarbons without molecular diffusion limitation. The conventional processes to synthesize Al-SBA-15 are time-consuming and often suffer from low “framework” Al contents. Herein, Al-SBA-15 microspheres are synthesized using the rapid and scalable microfluidic jet spray drying technique. They possess uniform particle sizes (45–60 μm), variable surface morphologies, high surface areas (264–340 m2/g), uniform mesopores (3.8–4.9 nm) and rich acid sites (126–812 μmol/g) and high acid strength. Their physicochemical properties are compared with the counterparts synthesized using traditional hydrothermal and evaporation-induced self-assembly methods. The spray drying technique results in a higher incorporation of aluminum (Al) atoms into the silica “framework” compared to the other two methods. The catalytic cracking efficiencies of 1,3,5-triisopropylbenzene (TIPB) on the Al-SBA-15 materials synthesized using the three different methods and nanosized ZSM-5 are compared. The optimal spray-dried Al-SBA-15 exhibits the best performance with 100 % TIPB conversion, excellent selectivity (about 75 %) towards the formation of deeply cracked products (benzene and propylene) and high stability. The catalytic performances of the spray-dried Al-SBA-15 with varying Si/Al ratios are also compared. The reasons for the different performances of the different materials are discussed, where the mesopores, high acid density and strength are observed to play the most critical role. This work might provide a basis for the synthesis of mesoporous rich metal-substituted silica materials for different catalytic applications.