Macromolecules incorporating photoactive species have become one of the most important topics in literature for the search of new materials with tunable properties. In particular, azobenzene-containing polymers have witnessed important developments in order to build up novel, smart materials for various useful purposes. The majority of these materials were completely organic macromolecules, however in recent years, azo dyes have been merged into organometallic polymers. Our group was one of the pioneers in this field via functionalization of organoiron macromolecules with aryl and hetaryl azo moieties. The combination of azo chromophore with organometallic macromolecules can tune the properties of the obtained polymers and increase the possibility of their applications in fields such as reversible optical storage systems, electrooptic modulators, labeling, photorefractive switches and biomedicine. Herein, we are highlighting the synthesis and characterization of various classes of highly colored organo and/or organoiron polymers and illustrating their possible applications.