The work is aimed at enhancing the Li+ ion-conduction properties of polymer electrolytes (PE) for thin-film solid-state batteries. The research exploits novel ideas of structuring ionically conducting polymers or molecular polyether building blocks with grafted magnetic nanoparticles with the use of magnetic field, in order to enhance ionic conductivity along oriented helical PE chains. The experimental route being tested is based on the chemisorption of thiolated PEO on core-shell gold-coated maghemite. It was found that casting, under a gradient magnetic field (GMF), of concentrated PEs containing very small concentration - 0.5%(w/w) dithiol-connected Fe2O3/Fe3O4-Au nanoparticles results in enhancement of the total ionic conductivity by more than an order of magnitude. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.