Abstract Widespread household use of solid fuels releases massive amounts of carbonaceous aerosols in developing countries. Assessment of their roles in meteorology and climate change is considered low confidence by the Intergovernmental Panel on Climate Change. Here, we leverage real‐world measurements to constrain the radiative absorption of light‐absorbing organic aerosols (i.e., brown carbon, BrC) from household coal and biofuel combustion within chemistry‐climate simulations. We determine the mass absorption efficiencies ranging from 0.7 to 3.2 m2 g−1 for coal and 2.1–5.8 m2 g−1 for biofuel, with an Absorption Ångström Exponent of about 5. Our improved simulations show that despite an ∼30% reduction from photobleaching, BrC radiative absorption still amounts to 16–49% of black carbon absorption in China, 2–7 times that simulated by commonly used parameterizations. Such importance of household‐derived BrC also exists in South Asia and Central Africa. Our results help reevaluate the intricate effects of anthropogenic emissions on weather and climate.