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Spherical carbon materials offer an optimal platform for this purpose, providing a distinctive combination of high packing density, isotropic electron\/ion transport, and structurally tunable hierarchical porosity. However, the field remains limited to fragmented and case\u2010specific studies, lacking a universal framework to decipher intricate \u201cstructure\u2010property\u201d relationships and overcome fundamental performance trade\u2010offs. To this end, this review proposes a pioneering \u201cprecursor, synthesis, structure, performance, and application\u201d paradigm for comprehensively analyzing spherical carbon materials. This review methodically explores how precursor engineering and synthesis strategies dictate critical structural parameters and elucidates the mechanistic links between these architectures and their resulting electrochemical performance. Furthermore, we critically examine key strategies\u2014such as hierarchical pore engineering, multiscale synergistic design, and interlayer\/spatial modulation\u2014that are instrumental in mitigating performance trade\u2010offs. These strategies are examined across a range of applications, including metal\u2010ion batteries, supercapacitors, Li\u2013S batteries, and fuel cells. Finally, the review delineates prospective research trajectories, emphasizing challenges in sustainable synthesis, advanced mechanistic understanding, and practical device integration. This framework is designed to accelerate the rational design and realization of next\u2010generation spherical carbon materials.<\/jats:p>","DOI":"10.1002\/smll.202514440","type":"journal-article","created":{"date-parts":[[2026,1,14]],"date-time":"2026-01-14T09:20:01Z","timestamp":1768382401000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Rational Design of Spherical Carbon Materials: Resolving Performance Trade\u2010Offs in Electrochemical Energy Storage"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-0224-0525","authenticated-orcid":false,"given":"Xinyu","family":"Liu","sequence":"first","affiliation":[{"name":"Shanxi Key Laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences  Taiyuan P. R. China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huihui","family":"Li","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Taiyuan University of Technology  Taiyuan P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guoli","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shanxi Key Laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences  Taiyuan P. R. China"},{"name":"College of Materials Science and Engineering Taiyuan University of Technology  Taiyuan P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaixi","family":"Li","sequence":"additional","affiliation":[{"name":"Shanxi Key Laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences  Taiyuan P. R. China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing P. R. 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