Metal catalysts are of great importance in the modern chemical industry. It is well-known that the structures of metal catalysts determine their properties. However, recent studies suggested that the structures of metal catalysts change dynamically under reaction conditions, resulting in the deactivation or activation of metal catalysts. This Review summarizes the latest research progresses in the structural reconstruction of metal catalysts via controlled-atmosphere transmission electron microscopy. The stateof-the-art research technologies and crucial factors affecting the nanosized metal catalyst reconstruction are discussed. Various types of reconstruction phenomena are reviewed, including sintering and dispersion, reshaping, composition evolution, surface reconstruction of metal oxides, and strong metal−support interactions. Moreover, recent studies of the structure−property relationship of metal catalysts are also reviewed. Finally, we highlight current challenges and provide the perspectives for future research of this topic. We hope this Review provides insights for the rational design of highperformance metal catalysts.