Metal organic frameworks (MOFs) are ideal fillers for preparing mixed matrix membranes (MMMs) because of their molecular sieving property. However, MOF nanoparticles are not easy to be dispersed, which limits their application in MMMs with high MOFs loading. In this study, highly dispersed ZIF-8 nanoparticles with diameter of around 50 nm were prepared by coating isophthalic dihydrazide (IPD) molecular layer onto their surfaces via coordination interaction (abbre. [email protected]). Benefiting from the highly stable and highly dispersed [email protected] solution, MMMs with high nanoparticles loading content and excellent uniformity are achieved. The modification of IPD on the surface of ZIF-8 nanoparticles greatly enhances the interfacial affinity between ZIF-8 as filler and 6FDA-Durene polyimide (PI) as polymer matrix under the interaction of strong hydrogen bond between them. Gas permeation results reveal that the H2 permeability of [email protected] mixed PI (PI/[email protected]) MMM with 45 wt% loading content is up to 8000 Barrer and the corresponding ideal selectivities of H2/CH4 and H2/N2 gas pairs are 15.1 and 13.0, which increase by 46.6% and 32.7%, respectively, comparing to those of ZIF-8 mixed PI (PI/ZIF-8) MMMs. The comprehensive separation performance of PI/[email protected] MMMs surpasses the 2008 Robeson’s upper bounds. The surface modification of IPD enhances the CO2 plasticization resistance property of PI/[email protected] MMMs from 21 bar to 30 bar. This study provides a facile and easy-operated strategy for the surface modification of MOF nanoparticles, and opens up a new way for the preparation of MMMs with high filler loading and good quality.