The concept of artificial intelligence (AI) is the transformation of inanimate objects into intelligent beings that can reason similarly to humans. Computer systems are capable of imitating a number of human intelligence functions, such as learning, reasoning, problem solving, speech recognition, and planning. In this regard, artificial intelligence applications have been developed to assist corporations and entrepreneurs in making business decisions. Hence, the aim of the study is to investigate the adoption of AI applications at the Vietnamese organizational level. Using the core structures of the technology–organization–environment (TOE), the theoretical model was constructed based on how technical and environmental elements influence companies’ technological innovation adoption decisions. Ten critical factors related to AI adoption are identified. To test the model, data were obtained from 193 senior managers who are directly in charge of information systems in both private and public companies in Vietnam. Subsequently, the Structural Equation Modeling (SEM) approach was used to analyze the data. The findings indicate that technical compatibility, relative advantage, technical complexity, technical capability, managerial capability, organizational readiness, government involvement, market uncertainty, and vendor partnership are significantly related to AI application adoption. Interestingly, the study results indicated that the relationship between organization size and AI adoption was not statistically significant. Therefore, the suggested adoption of the AI application could contribute to the existing research on the adoption of AI through the TOE. Finally, the significant government law implications and future research directions are further addressed.