Carbonaceous aerosols (or particles), which constitute one of most significant contribution of the atmospheric aerosols, are of worldwide concern due to their effects on environment, climate and human health. Two sub-fractions of total carbonaceous content of aerosols, Organic Carbon (OC) and Elemental Carbon (EC), not only differ in their origins but also in their effects on climate and human health. Radiocarbon (¹⁴C), as a radioactive isotope of carbon, has been proven to be a powerful tool of qualification and quantification of fossil and non-fossil contributions to OC and EC. This review introduces the principal and recent progress in the development of isolation method of different carbonaceous fraction for ¹⁴C measurement and compiles the results from ¹⁴C based source apportionment in China. Finally, the review concludes with some comments on current issues and future prospects using ¹⁴C as a source apportionment tool of atmospheric aerosols.