A study of the K-bentonites in the Doushantuo cap dolostones on the Yangtze Platform in South China would facilitate understanding the origin of the Marinoan cap dolostones and testing the snowball Earth hypothesis. To date, sporadic work has been conducted on the whole-rock geochemistry of the K-bentonites from the platform and slope of the Yangtze Platform, to preliminarily understand the genesis of the K-bentonites. However, a study of the whole-rock geochemistry of the K-bentonites from the basin and on zircon geochemistry of the K-bentonites from the entire Yangtze Platform has not been carried out. Therefore, the nature of the primary magmas, source and tectonic setting of the source volcanoes, and the episodes of source volcanic eruptions of the K-bentonites are unknown, which hinders unraveling the possible link between the sedimentary model of the Marinoan cap dolostone and the K-bentonites. Here, we perform a systematic study of the whole-rock and zircon geochemistry of the K-bentonites. The major and trace element concentrations of the K-bentonites and trace element contents in their volcanic zircons suggest that the primary magmas of the K-bentonites from the Jiuqunao and Heyu sections are different in nature. The same geochemical results indicate that the source volcanoes of all the K-bentonites may occur in the extensional setting on the northern margin of the Yangtze Block. Hf isotopic compositions of the volcanic zircons in the K-bentonites imply that the source magmas of the K-bentonites are mainly mantle-derived, and may have mixed with the crustal materials from the northern margin of the Yangtze Block. Based on the difference in whole-rock and zircon geochemistry of the K-bentonites from Heyu and Jiuqunao, two episodes of the source volcanic eruptions of the K-bentonites could be identified. The K-bentonite at Heyu most probably represents the record of the old episode, while that at Jiuqunao represents the record of the young one. The here proposed dual episodic deposition of K-bentonites within the Doushantuo cap carbonates holds potential significance to constrain 1) the duration of the cap carbonate deposition and 2) their genesis in potential slushball or snowball Earth environments.