Cost-effective metal-based nanostructured hybrids have been widely dedicated to potential energy storage and conversion applications. Herein, we develop a facile methodology for the synthesis of precise carbon-confined hybrid nanostructures by stereoselective assembly accompanied by catalytic pyrolysis. Polyacrylonitrile fiber films favors not only metal-polymer coordination, but also oriented assembly to ensure the well-defined nanostructure of the carbon hybrids. During chemical vapor deposition (CVD), cobalt-nanoparticle-catalyzed growth of carbon-nanotube branches driven by organic molecules (e.g. melamine) delivers hierarchical carbon hybrids. The resulting carbon hybrids exhibit outstanding electrochemical performance for metal-ion batteries, for example, a high specific capacity of 680 mAh g after 320 cycles (Li-storage) and 220 mAh g after 500 cycles (Na-storage) without decay.
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