In the last two decades, titanocene monochloride has been postulated as a monoelectronic transfer reagent capable of catalyzing an important variety of chemical transformations. In this Perspective, our contributions to this growing field of research are summarized and analyzed. Especially known have been our contributions in C-C bond formation reactions, hydrogen-atom transfer from water to radicals, and isomerization reactions, as well as the development of a catalytic cycle that has subsequently allowed the preparation of a great variety of natural terpenes. It is also worth mentioning our contribution in the postulation of this single-electron transfer agent (SET) as a new green catalyst with a broad range of applications in organic and organometallic chemistry. The most significant catalytic processes developed by other research groups are also briefly described, with special emphasis on the reaction mechanisms involved. Finally, a reflection is made on the future trends in the research of this SET, aimed at consolidating this chemical as a new green reagent that will be widely used in fine chemistry, green chemistry, and industrial chemical processes.