With the booming exploration and development of unconventional hydrocarbon resources in source rocks, the estimation of total organic carbon (TOC) content from well logs has become increasingly important because of the significance of TOC in the formation evaluation of those resources. In this paper, a new log overlay method is developed to estimate the TOC content of source rocks with excess radioactivity, but containing little or no potassium feldspar. Specifically, on the basis of previous results of log responses of source rocks, it is believed that the natural gamma ray (GR) log responses of source rocks in the applicable conditions are predominantly contributed by clay minerals and organic matter. A practical clay indicator is established to reflect the clay content using density and neutron logs. The indicator is effective not only in nonsource rocks that contain oil or water but also in source rocks. Furthermore, a new method was developed by overlaying the properly scaled clay indicator curve on the GR curve. In nonsource rocks, including clay-rich rocks and reservoirs saturated with oil or water, the two curves overlie each other, whereas a separation between the curves occurs in organic-rich source rocks. The separation between the curves was defined and expressed and can be used to calculate the TOC consecutively after careful calibration with core data. This method has been successfully applied to two shale gas plays with high-maturity kerogen in the Sichuan Basin, China. In addition, a source rock with low-maturity kerogen was used to verify the new method for its effectiveness, reliability, and widespread adaptability.