Silicic eruptive units can constitute a substantive component in flood-basalts-dominated large igneous provinces, but usually constitute only a small proportion of the preserved volume due to poor preservation. Thus, their environmental impact can be underestimated or ignored. Establishing the original volume and potential climate-sensitive gas emissions of silicic eruptions is generally lacking for most large igneous provinces. We present a case study for the ∼260 Ma Emeishan province, where silicic volcanic rocks are a very minor component of the preserved rock archive due to extensive erosion during the Late Permian. Modal and geochemical data from Late Permian sandstones derived from the province suggest that silicic volcanic rocks constituted some ∼30% by volume of the total eroded Emeishan volcanic source rocks. This volume corresponds to >3×104 km3 on the basis of two independent estimate methods. Detrital zircon trace element and Hf isotopic data require the silicic source rocks to be formed mainly by fractional crystallization from associated basaltic magmas. Based on experimental and theoretical calculations, these basalt-derived ∼104 km3 silicic eruptions released ∼1017 g sulfur gases into the higher atmosphere and contribute to the contemporaneous climate cooling at the Capitanian–Wuchiapingian transition (∼260 Ma). This study highlights the potentially important impact on climate of silicic eruptions associated with large igneous province volcanism.