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Introducing ZIF-8 into the PES-cSMM membranes played a pivotal role in the development of proton-conducting pathways and an effective methanol barrier. We employed dry-wet phase inversion techniques to fabricate PES-cSMM, finding that a 3 wt% cSMM content yielded optimal results. The resulting PES-cSMM exhibits impressive performance, with a 38% higher selectivity and a 95% greater methanol barrier compared to Nafion® 117. The imidazole-N-H linker in the terminal PES-cSMM/ZIF-8 promotes proton transport through a hydrogen bond chain, while the hydrophobic backbone acts as an effective methanol filter. As a result, PES-cSMM/ZIF-8 boasts a 13-fold higher water uptake than Nafion® 117 and achieves a 99% improvement in methanol sieving performance, a highly promising breakthrough for DMFC systems. Proton conductivity for the PES-cSMM/ZIF-8 immersion membrane reaches 19.5 × 10-3 Scm-1, comparable to Nafion® 117, which is 20.4 × 10-3 Scm-1. The structural flexibility of ZIF-8 within PES-cSMM facilitates efficient proton conduction, while the ZIF-8 cage acts as a robust methanol barrier. Computational analysis revealed covalent bonding within the PES-cSMM system. We characterized the chemical interactions in PES-cSMM/ZIF-8 using topology analysis, specifically the Atom in Molecules/Non-covalent analysis (AIM/NCI) technique. [Display omitted] • PES-cSMM made via dry-wet phase inversion; ZIF-8 added in-situ by growth immersion technique. • PES-cSMM/ZIF-8 shows promise in reducing methanol crossover, with good selectivity, stability, and proton conductivity for DMFC. • Proton transport occurs through non-covalent interactions with exposed sulfonic acid groups on the cSMMs within the membrane. • Computational findings suggest ZIF-8 interacts with methanol mainly via van der Waals forces. [ABSTRACT FROM AUTHOR]