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The contactless electric–field accomplishes particles alignment in solution allowing free solvent evaporation without electrochemical decomposition. Herein the nanoparticle Li1+xAlxGe2-x(PO4)3(LAGP) Z-direction (out-of-plane) alignment was driven by a contactless electric field within a cross-linked solid electrolyte of poly(ethylene oxide)/poly(ethylene glycol) diacrylate/lithium bis(trifluoromethylsulfonyl)imide (PEO/PEGDA/LiTFSI). The alignment and chain formation of nanoparticles was verified by scanning electron microscope combining with energy dispersive X-ray spectrometry. Benefiting from this Z-direction alignment, LAGP/PEO/PEGDA/LiTFSI membrane possesses enhanced ionic conductivity and improved flexibility. With 20 wt% LAGP loading, 2.7 times ionic conductivity was achieved in the Z- direction and 1.6 times elongation at breaking was obtained along the membrane surface after alignment. This contactless electrical field method is a new strategy to prepare polymer composite membrane with anisotropic property from solvent-containing system.