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The basic feature of polymers is their multi-order structure. Structure change at each level offers a possibility tomodify polymer properties and to develop new polymer materials. Therefore,novel polymer materials can be developed by tailoring their chain structure through chemical bonding among atoms, i.e., via the traditional molecular chemistry methods, e.g., polymerization of new monomer, controlling chain length (molecular weight and molecular weight distribution) and stereoregularity, copolymerization of different kinds of monomers, controlling sequence distribution,block of graft length of copolymer, etc., which have been the focus of polymer chemistry for several decades, as well as by tailoring specific supramolecular architecture using molecules as building block through intermolecular interactions, i.e., via supramolecular science methods, e.g., molecular self-assembly, intermacromolecular complexation, etc., which is a modern and fast-developing academic research field.This paper reports novel polymer materials prepared through intermacromolecular complexation,e.g., a new polymer solid electrolyte poly(metyl methacrylate-methacrylic acid)[P(MMA-MAA)]/poly(ethylene oxide) (PEO)/A2-LiClO4 developed by intermacromolecular complexation through hydrogen bonding, which has enhanced ambient ionic conductivity and fairly good mechanical and film-forming properties, a new polymer microcomposite poly(acrylonitrile-acrylamide-acrylic acid) [P(AN-AM-AA)]/poly(vinyl alcohol) (PVA) reinforced by the twin molecular chain microfibrils formed through intermacromolecular complexation of P(AN-AM-AA) with PVA through hydrogen bonding, which exhibits much better mechanical properties than its constituents and could be used to manufacture PVA based complexed fibers with higher modulus and better dyeability, a new polymer flooding agent poly(acrylamide-acrylic acid)[P(AM-AA)]/poly(acrylamide- dimethyldiallylammonium chloride) [P(AM-DMDAAC)] developed by intermacromolecular complexation of the oppositely charged polyions through Coulomb forces,which shows much higher viscosity and better resistance to temperature, shear rate and salt than its constituents, and has potential application in enhanced oil recovery.