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The paleoclimate during the Early Eocene in Maritime Antarctica is characterized by cool conditions without a pronounced dry season. Soils formed on volcanic material under such climate conditions in modern analogue environments are usually Andosols rich in nanocrystalline minerals without pedogenic smectite. The paleosols formed on volcanic material on King Georges Island are covered by basalts, dated by 6 new 40Ar/39Ar datings to 51–48 Ma, and are rich in smectite. A pedogenic origin of the smectites would suggest a semi-arid rather than a wet non-seasonal humid paleoclimate. To investigate the origin of the smectites in these paleosols we used X-ray diffraction and microscopic techniques. Minor mineralogical changes between the volcanic parent material and the paleosols and a homogenous distribution of smectites throughout the paleosol horizons indicate that these smectites were mainly inherited from the pyroclastic parent material, which was altered prior to surficial weathering. Nevertheless, the mineralogical properties, such as degree of crystallinity and octahedral site occupancy, of these smectites were modified during the ancient soil formation. Our findings highlight that trioctahedral smectites were a product of deuteric alteration of pyroclastic rocks and were progressively transformed to dioctahedral smectites during weathering in a soil environment on King George Island.