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Objective The effect of renin–angiotensin system inhibitors (RASIs) in patients with heart failure (HF) and atrial fibrillation (AF) remains unclear. This study aimed to investigate associations between RASI use and all-cause mortality and cardiovascular outcomes in patients with AF and HF. Methods Using data from the China Atrial Fibrillation Registry study, we included 938 patients with AF and HF with a left ventricular ejection fraction <50%. Cox regression models for RASIs vs. non-RASIs with all-cause mortality as the primary outcome were fitted in a 1:1 propensity score-matched cohort. A sensitivity analysis was performed by using a multivariable time-dependent Cox regression model. As an internal control, we assessed the relation between β-blocker use and all-cause mortality. Results During a mean follow-up of 35 months, the risk of all-cause mortality was similar in RASI users compared with non-users (hazard ratio: 0.92; 95% confidence interval: 0.67–1.26). Similar results were obtained in the sensitivity analysis. In contrast, β-blocker use was associated with significantly lower all-cause mortality in the same population. Conclusions RASI use was not associated with better outcomes in patients with AF and HF in this prospective cohort, which raises questions about their value in this specific subset. Trail Registration: ChiCTR-OCH-13003729.