Brittleness is important in the evaluation of the fracturing ability of shale reservoir and has a significant impact on shale gas exploration and development. This paper discusses the characteristics and controlling factors of brittleness of continental shale in the Da’anzhai Member of the Ziliujing Formation of Lower Jurassic age in the northeast Sichuan Basin. Continental shale lithofacies and their associations were grouped into four main rock types: clayey shale, silty shale, shell calcareous clayey shale, and silty clayey shale, characterized by the high clay content and local enrichment of carbonate minerals as a whole. Compared with the marine shale, the continental shale contained a low content of siliceous minerals, a high content of carbonate minerals, and a large number of shell limestone interlayers. Carbonate minerals play an important role in controlling the brittleness of continental shale. The shale interlayers were mainly shell limestone interlayers with a thickness of several centimeters and a large number of shell laminates with thicknesses of several millimeters were also observed. The shell laminates were mainly filled with calcite. Due to the dissolution process, a large number of bedding joints and corrosion joints were formed in the calcite shell layers. In the interlayers with a high shell content, a large number of microfractures developed. The energy consumption required for maintaining fracture expansion was lower after fracturing; the fractures greatly improved the reservoir’s brittleness.