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A novel insertable and pseudocapacitive Li+ ion material for highly ordered layered montmorillonite/carbon is explored in the present study. The commercially available protonated montmorillonite and 3,3′-diaminobenzidine act as starting materials to synthesize the layered material via hydrothermal intercalation, oxidative polymerization and carbonization. This method of preparing montmorillonite/carbon nanocomposite exhibits several advantages. To be specific, raw materials are low cost and naturally abundant; the montmorillonite can undergo proton exchange easily to form a permutable proton-type material, and the protons in the layered nanocomposite can be directly substituted by the polymerizable molecules (e.g., 3,3′-diaminobenzidine). Accordingly, a sheet-like montmorillonite/carbon layered nanocomposite is achieved with the carbon stacking on the montmorillonite substrate for the intercalation behavior. As revealed from the electrochemical results, montmorillonite/carbon nanocomposite can deliver a high reversible capacity of 1432 mA h g−1 at 50 mA g−1 and superior rate capacity of 920 mA h g−1 at 10 000 mA g−1 for the lithium ion battery. Furthermore, the full cell with LiFePO4 as cathode and montmorillonite/carbon as anode maintains 94% capacity retention over 50 cycles as well as high coulombic efficiency.