Over the last decade, carbon-based metal-free electrocatalysts (C-MFECs) have become important in electrocatalysis. This field is started thanks to the initial discovery that nitrogen atom doped carbon can function as a metal-free electrode in alkaline fuel cells. A wide variety of metal-free carbon nanomaterials, including 0D carbon dots, 1D carbon nanotubes, 2D graphene, and 3D porous carbons, has demonstrated high electrocatalytic performance across a variety of applications. These include clean energy generation and storage, green chemistry, and environmental remediation. The wide applicability of C-MFECs is facilitated by effective synthetic approaches, e.g., heteroatom doping, and physical/chemical modification. These methods enable the creation of catalysts with electrocatalytic properties useful for sustainable energy transformation and storage (e.g., fuel cells, Zn-air batteries, Li-O2 batteries, dye-sensitized solar cells), green chemical production (e.g., H2O2, NH3, and urea), and environmental remediation (e.g., wastewater treatment, and CO2 conversion). Furthermore, significant advances in the theoretical study of C-MFECs via advanced computational modeling and machine learning techniques have been achieved, revealing the charge transfer mechanism for rational design and development of highly efficient catalysts. This review offers a timely overview of recent progress in the development of C-MFECs, addressing material syntheses, theoretical advances, potential applications, challenges and future directions.