We report the lithium enrichment in the late Cretaceous Yetang Formation, located in the Shirenbei Basin, northeast of Guangdong Province. The Li2O content is greater than 0.2%, and can be a target for extracting lithium. Comprehensive crosssections of the Shirenbei Basin, geochemical analyses and lithofacies interpretation suggest that the lithium-enriched layers occur in shale, mudstone and siltstone, located in Middle-Upper Yetang Formation; lithium is mainly stored in clay minerals, whose formation is closely related to volcanic activities. It was initially interpreted as a volcanic-type lithium-rich clay deposit. The basin structure provides the environment for sedimentation and concentration of lithium. The layers containing enriched lithium are approximately 226 meters thick in total, and are in great potential for extracting lithium deposit. This discovery provides fclues on investigating large-scale lithium-rich clay deposits related to volcanic activities along the southeast coast of China.