Amidst global imperatives for sustainable energy and environmental remediation, carbon aerogels (CAs) present a transformative alternative to conventional carbon materials (e.g., activated carbon, carbon fibers), overcoming limitations of disordered pore structures, unmodifiable surface chemistry, and functional inflexibility. This review systematically examines CA-based electrochemical systems as its primary focus, analyzing fundamental charge-storage mechanisms and establishing structure–property–application relationships critical to energy storage performance. We critically assess synthesis methodologies, emphasizing how stage-specific parameters govern structural/functional traits, and detail multifunctional modification strategies (e.g., heteroatom doping, composite engineering) that enhance electrochemical behavior through pore architecture optimization, surface chemistry tuning, and charge-transfer kinetics acceleration. Electrochemical applications are extensively explored, including the following: 1. Energy storage: supercapacitors (dual EDLC/pseudocapacitive mechanisms) and battery hybrids. 2. Electrocatalysis: HER, OER, ORR, and CO₂ reduction reaction (CO₂RR). 3. Electrochemical processing: capacitive deionization (CDI) and electrosorption. Beyond this core scope, we briefly acknowledge CA versatility in ancillary domains: environmental remediation (heavy metal removal, oil/water separation), flame retardancy, microwave absorption, and CO₂ capture.

Supercapacitors have a rapid charge/discharge rate, long lifespan, high stability, and relatively acceptable cost, showing great potential in energy storage and conversion applications. However, the current cost-effective carbon-based electrodes have limited application owing to their low specific capacitance and unsatisfactory stability. In this regard, we herein prepare nitrogen-doped carbons by carbonizing a mixture of cotton pulp (CCP) and melamine to improve the specific capacitance by integrating pore (mesopore) and surface (oxygen-containing groups) modification with defect engineering via the carbonization process. Furthermore, the structural and morphological features of the resultant nitrogen-doped carbons are confirmed by various characterization techniques. Excitingly, the specific capacitance for nitrogen-doped CCP (CCPN1) with a 1 : 1 weight ratio of CCP and melamine is 642 F g⁻¹ at a current density of 0.5 A g⁻¹ in a three-electrode system, surpassing that of the reported carbon analogues and most metal-based materials to date. The stability test suggests that the specific capacitance of CCPN1 is maintained over 150 F g⁻¹ at a current density of 2 A g⁻¹ even over 5000 cycles. Therefore, the reported nitrogen-doped carbons from cotton pulp exhibit improved specific capacitance and stability, providing a new cost-effective carbon-based material for application in the energy storage field.