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In this work, innate free-standing and flexible anode composed of entangled N-doped carbon nanotubes (CNTs) is fabricated by a facile annealing method following a simple compression without needing any tedious processing operations. The well cross-linked CNTs of the resultant free-standing anode enable robust diffusion channels for lithium ions and high flexibility. Served as the anode in lithium-ion batteries (LIBs) without the utilization of binder and current collector, the fabricated free-standing electrode can deliver a reversible area capacity of 2.14mAhcm${}^{-2}$ at 1mAcm${}^{-2}$ with superior cycling stability and excellent rate capability. The obtained reversible area capacity for the fabricated free-standing electrode material is much higher than that of the commercial graphite anode ($\sim 0.6$mAhcm${}^{-2}$ at 1mAcm${}^{-2}$). Furthermore, the assembled full flexible battery utilizing the fabricated free-standing electrode also exhibits attractive performance and can substantially supply power for an electronic watch at flat and 180^∘ bending positions, indicating the promising application in flexible electronic devices.