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Advances in research and development of carbon-based metal-free electrocatalysts (C-MFECs) have provided potential alternatives to precious metal catalysts for various reactions important to renewable energy and environmental remediation. This timely but critical review provides an overview of recent breakthroughs (within the past 5 years or so) on C-MFECs in all aspects, including the design and regulation of intrinsic catalytic active sites, design and synthesis of carbon composite and hybrid carbon catalysts, mechanism understanding, and potential applications in clean energy storage and energy/chemical conversion. Current challenges and future opportunities in the field of metal-free carbon electrocatalysis are also discussed to provide forward-looking opportunities for their potential applications in various catalytic processes of practical significance.