The developing field of active, stimuli-responsive materials is in need for new dynamic architectures that may offer unprecedented chemomechanical switching mechanisms. Toward this goal, syntheses of polymerizable bipyridine ligands, bis(4-vinylbenzyl)[2,2′-bipyridine]-4,4′-dicarboxylate and N4,N4′-bis(4-vinylphenyl)-2,2′-bipyridine-4,4′-dicarboxamide, and a number of redox-active Ruthenium(II) and Iron(II) complexes with them are reported. Detailed characterizations by NMR, Fourier transform infrared spectroscopy, high-resolution mass-spectrometry, X-ray, and cyclic voltammetry show that the topology of these molecules allows them to serve as both comonomers and crosslinkers in polymerization reactions. Electronic properties of the ligands are tunable by choosing carboxylate-or carboxamido-linkages between the core and the vinylaryl moieties, leading to a library of Ru and Fe complexes with the M(III)/M(II) standard redox potentials suitable for catalyzing self-oscillating Belousov-Zhabotinskii (BZ) reaction. New poly(Nisopropylacrylamide)-based redox-responsive functional gels containing hydrophilic comonomers, which have been prepared using representative Ru bpy complexes as both a crosslinker and redox-active catalyst, exhibit a unique feature: their swelling/contraction mode switches its dependence on the oxidation state of the Ru center, upon changing the ratio of comonomers in the hybrid gel network. The BZ self-oscillations of such crosslinked hydrogels have been observed and quantified for both supported film and freestanding gel samples, demonstrating their potential as chemomechanically active modules for new functional materials.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.201704205.Ruthenium complexes with polypyridine ligand core, in particular, have occupied a significant place in this body of work, in big part due to the fact that they have been recognized to be useful in a wide variety of applications, which rely on their chemical stability, as well as a unique combination of photochemical, electrochemical, and photophysical properties. Among many potential applications that have emerged over the years, some recent examples include mononuclear water oxidation catalysis, [3] light-emitting electrochemical cells, [4] photoredox catalysis coupled with organocatalysis, [5] light-activated anticancer drugs, [6] and dye-sensitized solar cells. [7,8] Interest in integrating these valuable properties of polypyridine metal complexes into materials and devices gave rise to research in bipyridine-containing polymer ligands, as well as metallopolymers, coordination polymers, supramolecular polymers, and crosslinked polymer gels containing bipyridine moieties. [9] The targeted applications and research areas include, among others, electroluminescent, electrochromic, and photoluminescent materials, [9b,10,11] sensors, [9b,12] and chemomechanically active self-oscillating gels. [13][14][15][16] Interdisciplinary field of development and ...