The specific structure and diverse properties of hybrid organic-inorganic perovskite materials make them suitable for use in photovoltaic and sensing fields. In this study, environmentally stable organic-inorganic hybrid perovskite luminescent materials using Pb-MOF as a particular lead source were prepared using a mechanochemical method. Based on the fluorescence intensity of the MAPbBr3/MOF composite, the mechanized chemical preparation conditions of Pb-MOF were optimized using response surface methodology. Then, the morphological characteristics of the MAPbBr3/MOF composite at different stages were analyzed using electron microscopy to explore its transformation and growth process. Furthermore, the composite form of MAPbBr3 with Pb-MOF was studied using XRD and XPS, and the approximate content of MAPbBr3 in the composite material was calculated. Benefiting from the increase in reaction sites generated from the crush of Pb-MOF during mechanical grinding, more MAPbBr3 was generated with a particle size of approximately 5.2 nm, although the morphology of the composite was significantly different from the initial Pb-MOF. Optimal performance of MAPbBr3/MOF was obtained from Pb-MOF prepared under solvent-free conditions, with a milling time of 30 min, milling frequency of 30 Hz and ball-material of 35:1. It was also confirmed that the mechanochemical method had a good universality in preparing organic-inorganic hybrid perovskite/MOF composites.