Due to diverse properties complementary to their crystalline state, organic-inorganic metal halide hybrid (OIMH) glasses are drawing increasing attention. Nevertheless, the fundamental principles governing glass formation and crystallization in these materials remain elusive, significantly limiting their multifunctional applications. Here, high glass formation ability and tunable crystallization of glass are achieved through the regulation of intermolecular interactions. The π⋯π and C-H⋯π interactions among Bzmim