Graphene is the first and most famous member of two-dimensional (2D) nanomaterials family. Recently, other 2D materials, i.e., inorganic graphene analogues (IGAs) such as transition metal dichalcogenides (e.g., MoS2 and WS2), transition metal oxides (e.g., MnO2 and PbO2) and boron nitride (BN), also become the subjects of intense research. These 2D crystals are ideal fillers for high-performance polymer-matrix nanocomposites. Compared with graphene, IGAs are chemically more inert, and conventional carbon chemistry successfully employed on graphene is ineffective on them. Considering the abundant coordination atoms, such as S, O and N, present on IGAs, we envision a general way to chemically modify IGAs by metal ion coordination. In this study, we aim to establish a universal and effective strategy for the chemical modification, scalable production and hierarchical assembly of 2D materials through dynamic coordination interactions between 2D nanomaterials and polymeric ligands. The modified 2D materials can be stabilized in a wide range of organic solvents, including their nonsolvents, which largely improve their solution-phase processability. Moreover, dynamic coordination interactions are also employed to construct interfacial interactions between polymeric matrices and 2D nanomaterials (nanofillers), thereby developing robust, flexible polymeric super nanocomposites, thus opening up a new way to produce high-performance polymer-matrix nanocomposites.