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Self-assembly is one of the most sophisticated fabrication techniques for low-dimensional materials.Although great success has been achieved in preparing 0D and 1D materials by self-assembly of supramolecular polymer, the development of free-standing 2D supramolecular assemblies is far behind the blossoming 2D inorganic crystalline materials,such as graphene and its analogs.It is a great challenge to control the anisotropic 2D self-assembly and prevent the layer-layer stacking in the absence of template or interface.