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• Synthesis of CA-CNF by insulating block electrospinning & carbonization. • Formation of cross-aligned network even after heat treatment. • Faster reaction kinetics and regular electron pathway of CA-CNF. • High-rate cyclability of CA-CNF (259.4 mAh g−1 at 3000 mA g−1). The conventional use of metallic current collector in an electrochemical cell results in decreased loading of active materials and hence limited capacity in consideration of all the inactive current collector components. In response to this trend, a number of conductive, free-standing materials have been proposed as electrodes, which would act as both current collector and active materials. Here, in this study, we have firstly developed the cross-aligned carbon nanofiber (CA-CNF) for efficient Li storage, especially at high current densities. Using the insulating block electrospinning, the nanofibers can be aligned in a certain direction, where it is viable to fabricate cross-aligned nanofibers in a cost-effective and scalable manner. Attributed to faster kinetics and regular electron pathway arising from CA-CNF, it exhibits an excellent high-rate cyclability (259.4 mAh g−1 at a current density of 3000 mA g−1). This work builds up a milestone in suggesting a cross-aligned carbon nanofibrous network as efficient Li storage, which can also be applied to various electrode materials embedded cross-aligned conductive composite materials. [Display omitted] [ABSTRACT FROM AUTHOR]