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In this study, a novel MOFs-anchored-nanofiber framework (UiO-66-NH 2 @NFs) is designed via electrospinning. To hybridize with Nafion matrix, UiO-66-NH 2 @NFs/Nafion membranes with acid-base pairs are fabricated. In the framework, sulfonated poly(ether sulfone) (SPES) nanofibers with effective –SO 3 H groups serve as bonding platforms and UiO-66-NH 2 with –NH 2 groups act as co-reinforcement units tethering in nanofibers. As systematically studied and compared in membrane performance, the homogeneous UiO-66-NH 2 @NFs/Nafion membrane with a moderate UiO-66-NH 2 filler amount of 8 wt% present excellent performance on elevating proton conductivity of 0.27 S cm−1 (80 °C, 100% RH) and inhibiting methanol permeability of 7.54 × 10−7 cm2 s−1, respectively. The above superiorities can be attributed to the unique MOFs-anchored-nanofiber framework with balanced acid-base pairs. The interconnected UiO-66-NH 2 @NFs framework with hydrophilic SPES nanofibers and UiO-66-NH 2 offer consecutive proton transfer channels, making protons easily transfer via the hydration channels. Moreover, –NH 2 groups in UiO-66-NH 2 and –SO 3 H groups in matrix interact via acid-base pairs, which synergistically conducts protons via proton hopping channels in the membranes. Meanwhile, the good compatibility of UiO-66-NH 2 @NFs with Nafion matrix resulting from the tight electrostatically interactions between –NH 2 and –SO 3 H groups endow the hybrid membranes with suppressed methanol permeation and strengthened mechanical properties. Image 1 • UiO-66-NH 2 @NFs with acid-base pairs were built as proton-conducting highways. • Hybrid PEMs were prepared by incorporating UiO-66-NH 2 @NFs into Nafion matrix. • Acid-base interaction and consecutive proton conducting channels were well formed. • The hybrid PEMs exhibited high proton conductivity of 0.270 S cm−1 at 80 °C. [ABSTRACT FROM AUTHOR]