The 1963 eruption of Gunung Agung produced 0.95 km3 dense rock equivalent (DRE) of olivine±hornblende-bearing, weakly phyric, basaltic andesite tephra and lava. Evidence for magma mixing in the eruptive products includes whole-rock compatible and incompatible trace element trends, reverse and complex compositional zoning of mineral phases, disequilibrium mineral assemblages, sieve-textured plagioclase phenocrysts, and augite rims on reversely zoned orthopyroxene. Basalt magma mixed with pre-existing andesite magma shortly before eruption to yield basaltic andesite with a temperature of 1040–1100 °C at an assumed pressure of 2 kb, f O2>NNO, and an average melt volatile content (H2O±CO2) of 4.3 wt.%. Magma-mixing end members may have provided some of the S and Cl emitted in the eruption. Glass inclusions in phenocrysts contain an average of 650 ppm S and 3130 ppm Cl as compared with 70 ppm and 2220 ppm, respectively, in the matrix glass. Maximum S and Cl contents of glass inclusions approach 1800 and 5000 ppm, respectively. Application of the petrologic method to products of the 1963 eruption for estimating volatile release yields of 2.5×1012 g (Mt) of SO2 and 3.4 Mt of Cl released from the 0.65 km3 of juvenile tephra which contributed to stratospheric injection of H2SO4 aerosols on 17 March and 16 May, when eruption column heights exceeded 20 km above sea level. An independent estimate of SO2 release from atmospheric aerosol loading (11–12 Mt) suggests that approximately 7 Mt of SO2 was injected into the stratosphere. The difference between the two estimates can be most readily accounted for by the partitioning of S, as well as some Cl, from the magma into a water-rich vapor phase which was released upon eruption. For other recent high-S-release eruptions of more evolved and oxidized magmas (El Chichón, Pinatubo), the petrologic method gives values two orders of magnitude less than independent estimates of SO2 emissions. Results from this study of the Agung 1963 magma and its volatile emissions, and from related studies on eruptions of more mafic magmas, suggest that SO2 emissions from eruptions of higher-S-solubility magma may be more reliably estimated by the petrologic method than may those from more-evolved magma eruptions.