High-molecular-weight poly(ethylene oxide)s are utilized for a wide variety of different applications. Here we present a new strategy for the large-scale synthesis of modified metallosupramolecular poly(ethylene oxide)s on the basis of the metal-induced self-assembly of bis(2,2':6',2"-terpyrid-4'-yl)-poly(ethylene oxide)(179). The influence of different metal ions (cadmium(II), copper(II), cobalt(II), nickel(II), iron(II)) on the degree of polymerization and the resulting molecular weight were evaluated. Elaborated reaction conditions allow easy access to high-molecular-weight iron(H) coordination polymers via self-organization. The polymers were characterized in detail utilizing H-1 NMR, UV/vis spectroscopy, MALDI-TOF-MS, and viscosity measurements. The molecular weight was estimated on the basis of concentration-dependent viscosity measurements to about 80 000 g/mol. Furthermore, the morphology of the utilized telechelic bis(2,2':6',2"-terpyrid-4'-yl)-poly(ethylene oxide)(179) and the corresponding coordination polymer was investigated using atomic force microscopy. In particular, the influence of complex formation on the morphology was investigated.