Crystalline silica (mostly cristobalite) was produced by vapor-phase crystallization and devitrification in the andesite lava dome of the Soufriere Hills volcano, Montserrat. The sub-10-micrometer fraction of ash generated by pyroclastic flows formed by lava dome collapse contains 10 to 24 weight percent crystalline silica, an enrichment of 2 to 5 relative to the magma caused by selective crushing of the groundmass. The sub-10-micrometer fraction of ash generated by explosive eruptions has much lower contents (3 to 6 percent) of crystalline silica. High levels of cristobalite in respirable ash raise concerns about adverse health effects of long-term human exposure to ash from lava dome eruptions.