Electrochemical sodium storage and capture are considered an attractive technology owing to the natural abundance, low cost, safety, and cleanness of sodium, and the higher efficiency of the electrochemical system compared to fossil‐fuel‐based counterparts. Considering that the sodium‐ion chemistry often largely deviates from the lithium‐based one despite the physical and chemical similarities, the architecture and chemical structure of electrode materials should be designed for highly efficient sodium storage and capture technologies. Here, the rational design in the structure and chemistry of carbon materials for sodium‐ion batteries (SIBs), sodium‐ion capacitors (SICs), and capacitive deionization (CDI) applications is comprehensively reviewed. Types and features of carbon materials are classified into ordered and disordered carbons as well as nanodimensional and nanoporous carbons, covering the effect of synthesis parameters on the carbon structure and chemistry. The sodium storage mechanism and performance of these carbon materials are correlated with the key structural/chemical factors, including the interlayer spacing, crystallite size, porous characteristics, micro/nanostructure, morphology, surface chemistry, heteroatom incorporation, and hybridization. Finally, perspectives on current impediment and future research directions into the development of practical SIBs, SICs, and CDI are also provided. The key aspects of designing the structure and chemistry of carbon materials are comprehensively reviewed for applications such as sodium‐ion batteries, sodium‐ion capacitors, and capacitive deionization. The classification and features of carbon materials into graphitic and disordered carbons are described, as well as nanodimensional and nanoporous carbons, covering the correlation of structure and chemistry with electrochemical properties, and perspectives in electrochemical sodium‐ion storage and capture.