The construction of high‐quality carbon‐based energy materials through biotechnology has always been an eager goal of the scientific community. Herein, we first report juice vesicles bioreactors (JVBs) bio‐technology based on hesperidium (e.g., pomelo, waxberry, oranges) for preparation of carbon‐based composites with controllable components, adjustable morphologies, and sizes. JVBs serve as miniature reaction vessels that enable sophisticated confined chemical reactions to take place, ultimately resulting in the formations of complex carbon composites. The newly developed approach is highly versatile and can be compatible with a wide range of materials including metals, alloys, and metal compounds. The growth and self‐assembly mechanisms of carbon composites via JVBs are explained. For illustration, NiCo alloy nanoparticles are successfully in‐situ implanted into pomelo vesicles cross‐linked carbon (PCC) by JVBs, and their applications as sulfur/carbon cathodes for lithium‐sulfur batteries are explored. The well‐designed PCC/NiCo‐S electrode exhibits superior high‐rate properties and enhanced long‐term stability. Synergistic reinforcement mechanisms on transportation of ions/electrons of interface reactions and catalytic conversion of lithium polysulfides arising from metal alloy and carbon architecture are proposed with the aid of DFT calculations. Our research provides a novel biosynthetic route to rational design and fabrication of carbon composites for advanced energy storage.This article is protected by copyright. All rights reserved