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Gel polymer electrolyte (GPE) based on electrospun poly(vinylidene fluoride) (PVDF)/halloysite nanotube (HNT) nanocomposite non-wovens was synthesized and its suitability as a separator in lithium-ion battery (LIB) was explored. In this study, HNT played a key role in reducing the average diameter of the electrospun fibers and uplifted the porosity of the non-wovens thereby improving their electrolyte uptake. Due to a reduction in crystallinity and increased % porosity of the PVDF/HNT non-wovens, the ionic conductivity (1.77 mScm −1 ) and ionic transport across the separator were improved. Moreover, this GPE separator exhibited high tensile and puncture strength with negligible thermal shrinkage and a higher melting temperature compared with a commercially available separator, which is vital from the safety perspective. The cycling performance of Li/GPE/LiCoO 2 cell was evaluated and it exhibited a high capacity of 138.01 mAhg −1 with 97% coulombic efficiency for the initial cycle. The cell was stable and retained its high performance with little loss in capacity even after repeated charge-discharge cycles. Such a combination of high ionic conductivity, tensile strength with low thermal shrinkage is seen to be very rare in polymer-based separators. It is noteworthy that this novel GPE outperformed the commercial separator also in the cycle performance. POLYM. COMPOS., 40:2320-2334, 2019

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