Structural characterisation of proton-exchanged zeolites, prepared using ion-transfer at the liquid-liquid interface, is reported. Specifically, electrochemical exchange of protons for sodium with zeolites X and A is described: the structural integrity of the resultant materials was probed by solid-state NMR spectroscopy and temperature-dependent powder X-ray diffraction. It is shown that replacement of ca. 40 % of the Na + can be achieved using this approach for both zeolites; however, the results indicate that exchange is accompanied by significant structural degradation in the case of zeolite A, with proton exchange occurring at the amorphous regions of the sample. In contrast, zeolite X retains its structure, and the level of proton exchange is comparable with the highest levels reported using conventional chemical methods, highlighting the utility of the electrochemical approach.