Effective dispersion of fillers in the matrix is considered an efficient method to enhance the gas separation performance of hybrid membranes. In this study, metal-organic framework (MOF) nanoparticles dispersed in organosilica sol were successfully obtained by introducing urea into the precursor solution during the synthesis process. It was observed that the organosilica hybrid membrane, incorporated with urea-modulated MOF nanoparticles, exhibited a 3.3-fold increase in CO2/CH4 selectivities compared to the hybrid membrane incorporating non-modulated MOFs. These findings demonstrate the significant capability of urea-modulated MOFs to amplify the gas separation performance of hybrid membranes. This simple and feasible strategy can be widely used to produce various MOF-based membranes customized for diverse separation systems. (Yayun Zhao, Dechuan Zhao, Chunlong Kong, Yichao Lin, Xuezhen Wang, Liang Chen, Front. Chem. Sci. Eng. 2024, 18(2): 18)