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Herein a novel approach is introduced utilizing MOF\u2010derived nanoporous metal\/carbon composites as precursors to circumvent this traditional trade\u2010off. 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\u2010plane: 7311 S cm\u207b\u00b9, out\u2010of\u2010plane: 5541 S cm\u207b\u00b9) and excellent mechanical strength (flexural: 101.17\u00b15.73\u00a0MPa, compressive: 151.56\u00b12.53\u00a0MPa). Co nanoparticles act as autocatalysts and binders, promoting strong interlayer adhesion among highly graphitized graphene layers via spark plasma sintering. The strong nano\u2010interfaces between graphite and Co\u2010create 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.<\/jats:p>","DOI":"10.1002\/advs.202416210","type":"journal-article","created":{"date-parts":[[2025,1,9]],"date-time":"2025-01-09T06:31:51Z","timestamp":1736404311000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Breaking the Trade\u2010Off Between Electrical Conductivity and Mechanical Strength in Bulk Graphite Using Metal\u2013Organic Framework\u2010Derived Precursors"],"prefix":"10.1002","volume":"12","author":[{"given":"Yuqing","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fibers and Polymer Materials &amp; College of Materials Science and Engineering Donghua University  Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junzhuo","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fibers and Polymer Materials &amp; College of Materials Science and Engineering Donghua University  Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yinghan","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fibers and Polymer Materials &amp; College of Materials Science and Engineering Donghua University  Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8617-5025","authenticated-orcid":false,"given":"Qi","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fibers and Polymer Materials &amp; College of Materials Science and Engineering Donghua University  Shanghai 201620 China"},{"name":"Engineering Research Center of Advanced Glasses Manufacturing Technology Ministry of Education Donghua University  Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lianjun","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fibers and Polymer Materials &amp; College of Materials Science and Engineering Donghua University  Shanghai 201620 China"},{"name":"Engineering Research Center of Advanced Glasses Manufacturing Technology Ministry of Education Donghua University  Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1015-0371","authenticated-orcid":false,"given":"Wan","family":"Jiang","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fibers and Polymer Materials &amp; College of Materials Science and Engineering Donghua University  Shanghai 201620 China"},{"name":"Institute of Functional Materials Donghua University  Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,1,9]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaz8043"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-022-01292-4"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202308494"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202201867"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2017.06.010"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abc5555"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201603528"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202007513"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2022.11.083"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2020.08.011"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/accountsmr.4c00029"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-022-01425-9"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2020.04.003"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ceramint.2022.11.095"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2023.118295"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.3c11971"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.2c01952"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2023.142139"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2021.04.027"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/nl302870x"},{"key":"e_1_2_8_21_1","unstructured":"P. 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