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Proton exchang e membranes e xhibiting a well-org anized structure were successfully prepared by a novel self-assembling technique using surface- -charged latex nanoparticles as building blocks. The nanoparticles were synthe- sized in water by free-radical copolymerization. Free-standing membranes were obtained by casting the poly mer e mulsions followed by a cross-linking reac- tion. The acquired membrane exhibited a hig h proton condu ctivity of 0.04 S cm -1 with an ion exchange c apacity ( IEC) as low as 0.48 mmol g -1 . The e n- hanced proton conductivity is thought to be derived from the formation of a co- continuous ionic network for i on channels by the clo sely packed surface-char- ged latex nanoparticles, facilitating proton transportation in the membranes.