The ever‐growing portable electronics and electric vehicle draws the attention of scaling up of energy storage systems with high areal‐capacity. The concept of thick electrode designs has been used to improve the active mass loading toward achieving high overall energy density. However, the poor rate capabilities of electrode material owing to increasing electrode thickness significantly affect the rapid transportation of ionic and electron diffusion kinetics. Herein, a new concept named “sub‐thick electrodes” is successfully introduced to mitigate the Li‐ion storage performance of electrodes. This is achieved by using commercial nickel foam (NF) to develop a monolithic 3D with rich in situ heterogeneous interfaces anode (Cu3P‐Ni2P‐NiO, denoted NF‐CNNOP) to reinforce the adhesive force of the active materials on NF as well as contribute additional capacity to the electrode. The as‐prepared NF‐CNNOP electrode displays high reversible and rate areal capacities of 6.81 and 1.50 mAh cm−2 at 0.40 and 6.0 mA cm−2, respectively. The enhanced Li‐ion storage capability is attributed to the in situ interfacial engineering within the NiO, Ni2P, and Cu3P and the 3D consecutive electron conductive network. In addition, cyclic voltammetry, charge–discharge curves, and symmetric cell electrochemical impedance spectroscopy consistently reveal improved pseudocapacitance with enhanced transports kinetics in this sub‐thick electrodes.

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Enabling materials with distinct features toward achieving high-performance energy storage devices is of huge importance but highly challenging. Commercial carbon cloth (CC), because of its appealing chemical and mechanical properties, has been proven to be an excellent conductive substrate for active electrode materials. However, its performance is notably poor when directly used as an electrode in energy storage, due to its low theoretical capacity and surface area. Herein, we successfully endow the CC with enhanced storage capacity via formation of a π−π stacking interaction by integrating electrochemically activated CC (denoted CC/ACC) with biomass-derived carbon (BMDC) (denoted π-CC/ECC@BMDC). The π-CC/ECC@BMDC electrode displays excellent storage performance with a high capacity of 2.53 mAh cm −2 under 0.2 mA cm −2 when used as anode material for lithium ion batteries (LIBs). Due to the induction energy, the negatively charged molecules of the CC/ACC functional groups interact with the BMDC during carbonization, creating the π−π stacking interaction. Based on first-principles calculations, the structural design of the tri-layer carbon enables the movement of electrons around the π−π stacking interaction, which significantly facilitates rapid transportation of electrons, creates threedimensional (3D) ion tunnels for fast transportation of ions, and improves the electrode's mechanical and electronic properties.

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