This article presents new radiocarbon ages for the lavas, pyroclastic flow, and lahar deposits that originated from the Fugendake and Mayuyama volcanoes of the Younger Unzen Volcano, SW Japan. Nine charcoal samples were collected from the lavas and pyroclastic flow deposits, and 17 soil samples from the underlying volcanic-related products. This data set, together with previously published ages (thermoluminescence, K-Ar, fission track, and 14C), yielded new information about the timing of Late Pleistocene eruptions and an improved understanding of the evolution of the Fugendake and Mayuyama volcanoes. Fugendake Volcano started to build within the scar of Myokendake around 29 cal ka BP, and its eruption products spread over the flank of Myokendake. The remarkable eruptions of Fugendake Volcano included the lava and pyroclastic flow deposits around 22, 17, 12, and 4.5 cal ka BP. Subsequent historical eruptions occurred in AD 1663, 1792, and 1991–1995. Developed on the eastern extension of Fugendake Volcano, Mayuyama Volcano was active during the building stage of Fugendake at 4.5 cal ka BP. This study also identified a pumice eruption at ∼10 ka and 2 volcanic-related lahar deposits around 1.6 and 0.7 ka, which need to be addressed in future research.