Although three-dimensional (3D) host is effective in restricting Li dendrite growth, problems associated with the unstable electrode/electrolyte interphase becomes more severe due to increased interfacial area that is intrinsic of the 3D structures, being a major cause for the low Coulombic efficiency.While building a desirable solid electrolyte interphase (SEI) serves as an effective solution to improve the electrode/electrolyte interfacial stability, the 3D nature of the electrode makes the task challenging.Herein,we demonstrated the in-situ formation of SEI on chemically/structurally modified carbon cloth that is used as the 3D host.We shown that ZnS/ZnO nanotube arrays uniformly grown on the carbon cloth served as precursors for the in-situ formation of Li2S/Li2O/LiZn containing artificial SEI. While Li2S and Li2O are preferred components in SEI, Zn functions as lithiophilic site that guides the uniform lithium deposition.The present work shed light on effective design strategies for SEI formation on 3D electrode host with controllable SEI composition.