Self-care is important for improving the health outcomes of individuals with chronic heart failure (CHF). However, predictors of self-care behaviors remain unclear in Chinese society. The aims of this study were to explore predictors of self-care in Chinese patients with CHF and clarify the complex relationships between predictors and self-care behaviors guided by the Situation-Specific Theory of Heart Failure Self-Care. A cross-sectional study was conducted among individuals hospitalized with CHF in China. Person, problem, and environmental factors pertaining to self-care were collected by a questionnaire survey. Self-care was assessed by the Self-Care of Heart Failure Index version 6. Direct and indirect relationships between factors and self-care behaviors and the mediating role of self-care confidence were analyzed by the structural equation model. In total, 204 participants were involved in this study. The Situation-Specific Theory of Heart Failure Self-Care model demonstrated a good fit (root mean square error of approximation, 0.046; goodness of fit index, 0.966; normed fit index, 0.914; comparative fit index, 0.971). Inadequate self-care capabilities were common among Chinese patients with CHF. Person-related factors (female gender, higher monthly income and educational level), problem-related factors (severe New York Heart Association function class and better instrumental activities of daily living), and environmental factors (better social support and living in more developed areas) were significant predictors of better self-care behaviors ( P < .05). These associations were partly or fully mediated by self-care confidence. The Situation-Specific Theory of Heart Failure Self-Care can be used to guide research and practice in patients with CHF. Interventions and policies on promoting self-care in Chinese population living with CHF are encouraged, particularly for underserved populations.