Breaking the Trade‐Off Between Electrical Conductivity and Mechanical Strength in Bulk Graphite Using Metal–Organic Framework‐Derived Precursors

Abstract High‐performance bulk graphite (HPBG) that simultaneously integrates superior electrical conductivity and excellent strength is in high demand, yet it remains critical and challenging. Herein a novel approach is introduced utilizing MOF‐derived nanoporous metal/carbon composites as precursors to circumvent this traditional trade‐off. The resulting bulk graphite, composed of densely packed multilayered graphene sheets functionalized with diverse cobalt forms (nanoparticles, single atoms, and clusters), exhibits unprecedented electrical conductivity in all directions (in‐plane: 7311 S cm⁻¹, out‐of‐plane: 5541 S cm⁻¹) and excellent mechanical strength (flexural: 101.17±5.73 MPa, compressive: 151.56±2.53 MPa). Co nanoparticles act as autocatalysts and binders, promoting strong interlayer adhesion among highly graphitized graphene layers via spark plasma sintering. The strong nano‐interfaces between graphite and Co‐create critical bridges between graphene nanosheets, facilitating highly efficient electron migration and enhanced strength and stiffness of the assembled bulk nanocomposites. Leveraging these exceptional properties, practical demonstrations highlight the immense potential of the robust material for applications demanding superior electromagnetic interference shielding and efficient heating. An innovative approach, which effectively decouples electrical conductivity from mechanical properties, paves the way for the creation of HPBGs tailored for diverse application sectors.