Soil profiles of double-layer structure with Yellow-brown Earth (YBE) overlying Red Clay (RC) are commonly seen in the Xuancheng-Langxi-Guangde region, Anhui Province. Particle-size and geochemical characteristics of a selective YBE-RC soil profile in Langxi County, Anhui Province were studied. Results show that the YBE of the studied profile is quite coincident in particle-size composition and geochemical characteristics with that in Xuancheng and Jiujiang, and also the Xiashu Loess in Zhenjiang, Jiangsu Province, which strongly suggests that the YBE in the study areas shares the same provenance with the Xiashu Loess, widely distributed along the Yangtze Valley. The Langxi profile is vertically even in particle-size and geochemical characteristics, and also shows continuous transition between YBE and RC without any depositional interruption. This suggests that the underlying RC of the profile shares a similar origin with the YBE and the Xiashu Loess and was derived from typical aeolian-dust deposition. Compared with the YBE, however, the underlying RC is finer in particle-size and more intensively weathered. The transition from the RC to the YBE might record a great paleoclimatic change at the early stage of the Late Pleistocene, when the Last Interglacial ended and the Last Glacial began. However, more work needs to be done to find some irrefutable chronological evidence.