Three‐dimensional carbon nanotube/graphene sandwich structures with CNT pillars grown in between the graphene layers have been developed by chemical vapor deposition. The special structure endows the high‐rate transportation of electrolyte ions and electrons throughout the electrode matrix, resulting in excellent electrochemical performance of this hybrid material.

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A hybrid chemically converted graphene nanosheet/Ni 2+ /Al 3+ layered double-hydroxide (GNS/LDH) composite for supercapacitor material has been fabricated by a hydrothermal method. Scanning electron microscopy and transmission electron microscopy results reveal that Ni 2+ /Al 3+ LDH platelets homogeneously grew onto the surfaces of the GNSs as spacers to keep the neighboring sheets separate. Electrochemical properties were characterized by cyclic voltammetry, galvanostatic charge/discharge measurements, and electrochemical impedance spectroscopy. The composite exhibits a maximum specific capacitance of 781.5 F/g and excellent cycle life with an increase of the specific capacitance of 38.07% after 50 cycle tests. Even after 200 cycle tests, the increase of the capacitance is 22.56% compared with the initial capacitance.

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