Radiocarbon (14C) measurement of water-soluble organic carbon (WSOC) in ambient aerosols is a quantitative tool for unambiguously distinguishing fossil and non-fossil sources. In this study, a fast and reliable method for measuring 14C in micro-scale (μg) WSOC aerosol samples is successfully developed, which includes three steps: (1) extraction (2) freeze drying, and (3) online 14C analysis of CO2 from WSOC combustion. Procedure blanks are carefully assessed by measuring high-purity water and reference materials. Accurate 14C results could be obtained for WSOC with only 10μgC, and thus the potential applications are substantially broadened because much less filter material is needed compared to previous reported methods. This method is applied to aerosols samples collected during winter from Switzerland and China. The results demonstrate that non-fossil sources are important if not dominant contributors of WSOC. These non-fossil components are consistently enriched in WSOC compared to bulk OC and water-insoluble OC for all samples, due to high water solubility of primary and secondary biomass burning aerosols. However, the presence of fossil WSOC is still considerable indicating a substantial contribution of secondary OC (SOC) formed from precursors emitted by fossil emissions. Larger fossil contributions to WSOC is found in China than in Switzerland and previously reported values in Europe, USA and South Asia, which may be attributed to higher fossil-derived SOC formation in China.