AbstractLong‐term exposure to ambient fine particulate matter (PM_2.5) is the second leading risk factor of premature death in Sub‐Saharan Africa. We use GEOS‐Chem to quantify the effects of (a) trash burning, (b) residential solid‐fuel burning, and (c) open biomass burning (BB) (i.e., landscape fires) on ambient PM_2.5 and PM_2.5‐attributable mortality in Africa. Using a series of sensitivity simulations, we excluded each of the three combustion sources in each of five African regions. We estimate that in 2017 emissions from these three combustion sources within Africa increased global ambient PM_2.5 by 2%, leading to 203,000 (95% confidence interval: 133,000–259,000) premature mortalities yr⁻¹ globally and 167,000 premature mortalities yr⁻¹ in Africa. BB contributes more ambient PM_2.5‐related premature mortalities per year (63%) than residential solid‐fuel burning (29%) and trash burning (8%). Open BB in Central Africa leads to the largest number of PM_2.5‐attributed mortalities inside the region, while trash burning in North Africa and residential solid‐fuel burning in West Africa contribute the most regional mortalities for each source. Overall, Africa has a unique ambient air pollution profile because natural sources, such as windblown dust and BB, contribute strongly to ambient PM_2.5 levels and PM_2.5‐related mortality. Air pollution policies may need to focus on taking preventative measures to avoid exposure to ambient PM_2.5 from these less‐controllable sources.