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Grounded electrical-source airborne transient electromagnetics (GREATEM), a type of semi-airborne electromagnetics, was used to examine Aso Volcano in south-west Japan, to verify its applicability to surveying deep subsurface resistivity structures. Comparison of the GREATEM resistivity values with those of ground-based transient electromagnetics (TEM) data, repeated GREATEM survey results at the same and different flight heights, and lithologic descriptions indicated that GREATEM can successfully identify underground structures as deep as ~800 m in rugged mountainous areas. An active volcanic region (Naka-Dake crater) was mapped as a low-resistivity zone from the surface to a depth of 100 m. This low-resistivity zone extended to the west-north-west, implying future volcanic activity in this area. Therefore, the GREATEM method is useful for surveying deep structures in large, inaccessible areas, such as volcanic provinces, in a quick, cost-effective way.