We report the synthesis of ZnO nanostructures via electrodeposition onto films of polypyrrole (PPy) obtained by an electroless method from an aqueous suspension of PPy nanosheets. The PPy nanosheets are initially prepared in hexagonal oil-in-water (o/w) swollen liquid crystal (SLC) to provide the lamellar structure required to achieve further formation of a smooth electrode by an electroless process. The PPy particles can be easily extracted and transferred into an aqueous suspension that can be stored for months until its final use. The aqueous suspension of PPy is further spin-coated onto a glass or silicon substrate to form a flat thin film. These films exhibit a significant conductivity that allows further growth of various zinc oxide nanostructures by electrodeposition.