Empowered by blockchain and Web3 technologies, decentralized autonomous organizations (DAOs) are able to redefine resources, production relations, and organizational structures in a revolutionary manner. This article aims to reanalyze DAOs from the perspectives of organization and operation, and provide a more precise definition of DAOs as Decentralized Autonomous Organizations and Operations. Based on this, the fundamental principles and requirements of DAOs are explained, while the infrastructure based on cyber–physical–social system (CPSS) and parallel intelligence, as well as the supporting technologies, such as digital twins, metaverse, and Web3, are discussed. Besides, a five-layer intelligent architecture is presented, and the closed-loop equation and new function-oriented intelligent algorithms are also proposed. Moreover, the governance mechanisms from the individual, organizational and social perspectives are discussed, and the incentive mechanisms for the human, robot, and digital human are analyzed. This article can be regarded as a stepping stone for further research and developments of DAOs.