This study developed and empirically tested a model to predict the factors affecting patients' behavioral intentions to use a mobile health education website. It explored the behavioral intention to use a mobile health education website from the perspective of consumers by extending the Unified Theory of Acceptance and Use of Technology 2 model with the addition of mobile self-efficacy (M-SE), use motivation, and mobile literacy as moderators. For this purpose, variance-based structural equation modeling was used to analyze data collected from a sample of 1,649 patients at a hospital in Taoyuan, Taiwan. Partial least squares regression was used for model and hypothesis testing. The results revealed that (1) performance expectancy, effort expectancy, social influence, facilitating conditions, and habit were key predictors of the behavioral intentions of patients to use a mobile health education website; (2) M-SE had positive associations with effort expectancy; (3) use motivation was a significant determinant of both performance expectancy and effort expectancy; and (4) mobile literacy had a significantly negative moderating effect on the relationship between performance expectancy and behavioral intention. Our findings serve as a reference for the promotion of mobile health education in hospitals.