Imidazole moieties play an important role not only in biomacromolecules, such as DNA, RNA, proteins and enzymes, but also in many other useful substances, e.g. in vitamins and pharmaceuticals. Furthermore, synthetic macromolecules with imidazole groups have also gained broad interest on the basis of the unique chemical structure and properties of such polymers, on the one hand. On the other hand, amphiphilic polymer co-networks (APCN), composed of chemically bonded, otherwise macroscopically immiscible, polymer chains, have attracted broad interest in recent years. Moreover, APCNs with a poly(N-vinylimidazole) (PVIm) hydrophilic component offer exceptional opportunities for obtaining a variety of specialty nanostructured materials with unprecedented structural and property features. This Chapter overviews the latest findings related to synthesis principles, nanostructured morphologies with bicontinuous (co-continuous) nanophases in broad composition ranges, fundamental properties, nanohybrids and application possibilities, ranging from catalysis to antibacterial hybrid materials, of PVIm-based co-networks with hydrophobic poly(tetrahydrofuran) and polyisobutylene macromolecular crosslinkers, i.e. poly(N-vinylimidazole)-l-poly(tetrahydrofuran) (PVIm-l-PTHF) and poly(N-vinylimidazole)-l-polyisobutylene (PVIm-l-PIB) co-networks.