Quinone-containing materials have attracted significant attention for energy storage and electroswing carbon capture. Tailored redox-responsive core–shell particles are obtained in the present work via semicontinuous starved-feed emulsion polymerization and subsequent postmodification strategies with redox-responsive quinone moieties. The use of glycidyl methacrylate within the shell material offers the possibility of a ring-opening reaction with the redox-responsive 2-aminoanthraquinone (2-AAQ), which possesses a high affinity toward electrophilic carbon dioxide. The successful preparation of monodisperse particles, an essential prerequisite for colloidal self-assembly, was investigated by dynamic light scattering and transmission electron microscopy. The presence of reactive epoxy functionalities was achieved by the ring-opening reaction with the Preussmann reagent. Postsynthesis modification was investigated using X-ray photoelectron spectroscopy and cyclic voltammetry measurements. The redox-responsive core–shell particles were subjected to the melt-shear organization technique to prepare free-standing opal films featuring structural colors. The monodisperse 2-AAQ-containing particles were investigated for self-assembly inside conductive carbon felts, and their electrochemically mediated carbon capture capabilities were studied.