Volcanic-ash clouds can be fed by an upward-directed eruption column (Plinian column) or by elutriation from extensive pyroclastic flows (coignimbrite cloud). There is considerable uncertainty about which mechanism is dominant in large-scale eruptions. Here we analyze in a novel way a comprehensive grain-size database for pyroclastic deposits. We demonstrate that the Mount Pinatubo climactic eruption deposits were substantially derived from coignimbrite clouds, and not only by a Plinian cloud, as generally thought. Coignimbrite ash-fall deposits are much richer in breathable <10 μm ash (5–25 wt%) than pure Plinian ash at most distances from the source volcano. We also show that coignimbrite ash clouds, as at Pinatubo, are expected to be more water rich than Plinian clouds, leading to removal of more HCl prior to stratospheric injection, thereby reducing their atmospheric impact.