Exfoliation is a common route to synthesize 2D materials, such as monolayered and fewlayered nanosheets. However, it is not easy to control the breaking-down process. The repsent work shows a new exfoliation strategy for generation of nanosheets from soft layered composites in high yield. Soft layered composites of inorganic hosts and organic guests are exfoliated into nanosheets in organic dispersion media. A simple yield-prediction model is constructed on small-scale our own experimental data by sparse modeling, a data-scientific approach, combined with chemical perspective.