The aim of this work is to improve the electrochemical performance of lithium-ion batteries by developing an inorganic-polymer gel electrolyte and anode electrode, which both use helical mesoporous silica nanofibers (HMSFs) as the skeletons. Based on this design, the electrolyte/anode interphase is naturally integrated, which consequently show excellent properties in electrochemical measurements. The HMSFs incorporated into P(VDF-HFP) matrix to form the electrolyte membranes (named as NPCGE) exhibit high thermal stability (up to 372 ℃), wide electrochemical window (5.30 V), and high room temperature ionic conductivity (1.2 × 10−3 S cm−1). Meanwhile, helical mesoporous silica/Fe-N-doped carbon composite nanofibers (HMSFs@Fe-N-C) was fabricated by carbonizing Fe-adsorbed resin/silica/gel composites and then acted as the anode material in lithium-ion batteries (LIBs). The assembled HMSFs@Fe-N-C|NPCGE|Li cell show a high specific capacity around 1290 mAh g−1 over 500 cycles at a current density of 0.3 A g−1 and excellent rate performance, which was not only ascribed to the special composition and nanostructure of the electrolyte and electrode materials, but also to the benign interfacial contacts.