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 2.14[Formula: see text]mAh[Formula: see text]cm[Formula: see text] at 1[Formula: see text]mA[Formula: see text]cm[Formula: see text] 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 ([Formula: see text][Formula: see text]mAh[Formula: see text]cm[Formula: see text] at 1[Formula: see text]mA[Formula: see text]cm[Formula: see text]). 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.
