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Here, the concept of thick electrode is utilized to design a-17 mm three-dimensional (3D) all-carbon frameworks with remarkable structural stability as high-areal-capacity anode for lithium-ion batteries (LIBs). The framework involves the rational design of graphite fibers (GFs) bonded with pyrolytic carbon (PC) and graphite nanoplatelets (GNP), offering a unique architecture and a scalable production approach. The as-fabricated 3D-GF/PC/GNP electrode with a high mass loading of ≈30 mg cm−2 can deliver an unexpected high initial and reversible areal capacity of 23.53 and 11.63 mA h cm−2 at current density of 2.0 mA cm−2, impressive rate performance and cyclic stability. Both theoretical simulations and experimental analyses show that the excellent performance of the electrode can be attributed to the incorporation of GNP that modulates the electronic conductivity of the framework, enabling easier Li-ion intercalation/deintercalation pathway to promote the pseudocapacitive and surface adsorption Li-ion storage.

The “in-contact” mesophase spheres were obtained successfully by separating from mesophase sphere-containing pitches at a relatively low temperature of 220 °C using high-temperature centrifugation. The optical and scanning electron microscopies were employed to examine the characteristics of mesophase pitch samples. The results indicated that strong interactions between mesophase spheres started at relatively low temperature, with the contact point(s) occurring three dimensionally around spheres. The mesophase layers between different spheres appeared to dock with each other behind the scene, as these spheres came close enough and their lamellae at the contact point were orientated parallel with each other.