Featured with the attractive properties such as large surface area, unique atomic layer thickness, excellent electronic conductivity, and superior catalytic activity, layered metal chalcogenides (LMCs) have received considerable research attention in electrocatalytic applications. In this review, the approaches developed to synthesize LMCs‐based electrocatalysts are summarized. Recent progress in LMCs‐based composites for electrochemical energy conversion applications including oxygen reduction reaction, carbon dioxide reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, overall water splitting, and nitrogen reduction reaction is reviewed, and the potential opportunities and practical obstacles for the development of LMCs‐based composites as high‐performing active substances for electrocatalytic applications are also discussed. This review may provide an inspiring guidance for developing high‐performance LMCs for electrochemical energy conversion applications.