The chemical extraction of soil organic carbon (SOC) fractions from soils often does not produce satisfactory results for radiocarbon dating. In this study, a sequential pyrolysis technique was investigated. The soil was pyrolyzed at temperatures of 200, 400, 600, and 800 °C to partition organic carbon into pyrolytic volatile (Py-V) and pyrolytic residue (Py-R) fractions. The preliminary results show that the 14C dates of both fractions become progressively older as the pyrolysis temperature is increased. In addition, the ages of the Py-V fractions are consistently younger than the corresponding Py-R fractions extracted at the same temperature. Experimental results of known-age paleosol samples indicate that the Py-V fractions obtained between 600 and 800 °C yield the most reliable ages. This technique provides a new approach to improve the accuracy of 14C dating of loess-paleosol sequences.