Precise Tailoring of Unprecedent Layered Perovskite‐Type Heterostructure Ferroelectric via Chemical Molecular Scissor

. This motif is self-assembled by layer-by-layer clipping of rigid prototype sheets, using extra neopentylamine as a molecular chemical scissor. Unlike epitaxial growth, such a molecule-level stacking facilitates the growth of heterostructure single crystals. Combining its strong ferroelectricity and inherent anisotropy, crystal-based device of 1 exhibits an ultrahigh polarized-light sensitivity up to ~37 in self-powered mode, being the highest level of 2D perovskite ferroelectric family. Our work will facilitate the further development of ferroelectric materials for optoelectronic device applications.