for the LIBs to develop advanced anode materials with high specific capacity and long-cycle life. Recently, transition metal oxides, [4][5][6] sulfides, [7][8][9] nitrides, [10][11] and phosphides [12][13][14][15] have attracted extensive attention by virtue of their high theoretical capacity. Among them, transition metal phosphides (TMPs) are more suitable as LIBs anode materials by having a lower potential for lithium insertion, smaller voltage lag, and higher theoretical capacity. [16][17][18] Additionally, the lithiation products (Li 3 P) of TMPs show higher Li ionic conductivity (10 −4 S cm −1 ) than Li 2 O (5 × 10 −8 S cm −1 ) and Li 2 S (10 −13 S cm −1 ) at room temperature, which is beneficial for reducing the polarization. [19,20] To date, various phosphides have been reported, such as FeP, [21] MoP, [22] and CoP. [23,24] Among these candidates, CoP shows great potential for practical applications as an anode material because of its high theoretical capacity (894 mAh g −1 ) and low lithiation potential (≈0.6 V vs Li/Li + ). [25,26] Nevertheless, CoP still face the challenges of low conductivity, large volume expansion, and serious agglomeration, which inevitably restrict its rate and cycling performance. [24,25,27] In addition, the presence of inactive binders in traditional rigid electrodes based on slurry coating causes many invalid interfaces and poor contact of active material with the current collector, which leads to exfoliation of the active material from the current collector and poor kinetics during charge/discharge. [28,29] To overcome these challenges, many strategies have been proposed to achieve high-performance CoP anodes. First, the nanoscale design of CoP should effectively reduce the electron/ ion transport paths, such as nanowires, [27] nanorods, [25,26,30] nanoparticles. [23,31] Second, directly growing these nanostructures on conductive substrates to construct a binder-free electrode can effectively improve the electrochemical performance of the anode. [32][33][34] For example, Yang et al. successfully prepared a CFC@Ni 5 P 4 electrode via directly synthesizing Ni 5 P 4 on the carbon fiber cloth (CFC), which exhibited the best electrochemical performance compared to P-Ni 5 P 4 electrodes based on slurry coating. [35] Such binder-free structural design has the following advantages: i) the direct contact between the conductive substrates and the active materials is conducive to improve Cobalt phosphide (CoP) is considered as one of the most promising candidates for anode in lithium-ion batteries (LIBs) owing to its low-cost, abundant availability, and high theoretical capacity. However, problems of low conductivity, heavy aggregation, and volume change of CoP, hinder its practical applicability. In this study, a binder-free electrode is successfully prepared by growing CoP nanosheets arrays directly on a carbon cloth (CC) via a facile one-step electrodeposition followed by an in situ phosphorization strategy. The CoP@CC anode exhibits good interfacial bonding between the CoP and CC, whi...