We propose a novel material/electrode design formula and develop an engineered self-supporting electrode configuration, namely, silicon nanoparticle impregnated assemblies of templated carbon-bridged oriented graphene. We have demonstrated their use as binder-free lithium-ion battery anodes with exceptional lithium storage performances, simultaneously attaining high gravimetric capacity (1390 mAh g(-1) at 2 A g(-1) with respect to the total electrode weight), high volumetric capacity (1807 mAh cm(-3) that is more than three times that of graphite anodes), remarkable rate capability (900 mAh g(-1) at 8 A g(-1)), excellent cyclic stability (0.025% decay per cycle over 200 cycles), and competing areal capacity (as high as 4 and 6 mAh cm(-2) at 15 and 3 mA cm(-2), respectively). Such combined level of performance is attributed to the templated carbon bridged oriented graphene assemblies involved. This engineered graphene bulk assemblies not only create a robust bicontinuous network for rapid transport of both electrons and lithium ions throughout the electrode even at high material mass loading but also allow achieving a substantially high material tap density (1.3 g cm(-3)). Coupled with a simple and flexible fabrication protocol as well as practically scalable raw materials (e.g., silicon nanoparticles and graphene oxide), the material/electrode design developed would propagate new and viable battery material/electrode design principles and opportunities for energy storage systems with high-energy and high-power characteristics.

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