Designing Ni-based catalyst with high performance is one of the most important challenges for operation of practical steam-methane reforming (SMR) processes. We report control of the textural properties of commercial alumina ball for Ni-supported catalysts in SMR. The textural properties of the commercial Al2O3 sphere are successfully controlled by aqueous HCl treatment for elongated periods. The pore diameters and pore volumes of the controlled alumina supports are finely tuned by varying the HCl treatment period. The catalytic activity of the corresponding Ni-supported alumina is significantly enhanced with increasing HCl treatment period on alumina ball. The alumina supports with longer HCl treatment period have larger pore size and bigger pore volume, and the corresponding Ni-Alumina catalysts exhibited higher catalytic activity at even higher space velocity, due to the increased intraparticle diffusion of reactant molecules inside the catalyst. Ni-supported alumina catalyst prepared by using alumina support treated with HCl for 18 h showed the largest pore size and pore volume, revealing enhanced catalytic activity in terms of CH4 conversion and H2 yield. It showed the well-maintained activity without any further deactivation in both continuous operation for 24 h and cyclic operation at different WHSV conditions.