Gondwana, comprising >64% of the present-day continental mass, is home to 33% of Large Igneous Provinces (LIPs) and is key to unravelling the lithosphere–atmosphere system and related tectonics that mediated global climate shifts and sediment production conducive for life on Earth. Increased recognition of bimodal LIPs in Gondwana with significant, sometimes subequal, proportions of synchronous silicic volcanic rocks, mostly rhyolites to high silica rhyolites (±associated granitoids) to mafic volcanic rocks is a major frontier, not considered in mantle plume or plate process hypotheses. On a δ¹⁸O v. initial ⁸⁷Sr/⁸⁶Sr plot for silicic rocks in Gondwana LIPs there is a remarkable spread between continental crust and mantle values, signifying variable contributions of crust and mantle in their origins. Caldera-forming silicic LIP events were as large as their mafic counterparts, and erupted for a longer duration (>20 myr). Several Gondwana LIPs erupted near the active continental margins, in addition to within-continents; rifting, however, continued even after LIP emplacements in several cases or was aborted and did not open into ocean by coeval compression. Gondwana LIPs had devastating consequences in global climate shifts and are major global sediment sources influencing upper continental crust compositions. In this Special Publication, papers cover diverse topics on magma emplacements, petrology and geochemistry, source characteristics, flood basalt–carbonatite linkage, tectonics, and the geochronology of LIPs now distributed in different Gondwana continents.