Historical relics of Jurassic sandstones in southwest China have been subjected to weathering damage. Exfoliation, characterized by the detachment of multiple thin stone layers sub-parallel to the stone surface, is common in sandstone heritage sites. However, its mechanism of action remains poorly understood. In this study, a conceptual model of exfoliation is drawn from the literature and field investigations. To quantitatively determine the exfoliation mechanism, a range of non-destructive field-based methods (surface hardness, water absorption test, roughness, and amplitude of residual spalling layers) and laboratory analyses (scanning electron microscopy (SEM) and X-ray diffraction (XRD)) are adopted as weathering agents for separated detachments. In addition, the grain and pore sizes of weathering products are analyzed using digital image techniques. The results show that the roughness, water absorption coefficient, and pore size in sandstone surfaces increase from the inner layer to the outer layer, and their hardness and grain size decrease, respectively. The proportions of quartz, dolomite, and illite increases from the interior to the exterior, whereas the proportion of feldspar decreases correspondingly. The residual column strip structure derived from feldspar alteration and a mixed montmorillonite-illite mineral layer can be observed in the SEM images. It can be inferred from surviving environmental analysis that comprehensive actions from solar radiation, acid rain attack and capillary rise lead to sandstone exfoliation. In addition, the alteration of feldspar plays an important role during sandstone exfoliation. The results of this study enhance our understanding of the exfoliation of the Jurassic sandstone of the Chongqing Danzishi rock carvings in China.