The precise control of primary reactions in solutions is one of the most significant steps for the nanoscale design of inorganic solids in multidisciplinary fields. However, further growth of the inorganic species to give bulkier species disturbs such designs. The surfactant-assisted synthesis of mesoporous materials is a good strategy for addressing such concerns because pores formed by supramolecularly mediated processes are surrounded by nanometer-sized continuous frameworks. Many experiments are generally conducted to optimize the reaction conditions for the synthesis of highly ordered mesostructures. Herein, to minimize such trial-and-error efforts, a new and practical concept is proposed for the precise design of porous materials. By adjusting the reactivity between bisphosphonates and metal sources through molecular design of the starting bisphosphonate compound, it was possible to synthesize mesoporous films with unique compositions by a surfactant-assisted approach.