Historical examinations of the alchemical thought of Carl Jung have hitherto focused on the shortcomings of his historiography and its applications, largely neglecting the fundaments, formation, and sequence of his alchemical findings within the context of his psychological research: a deficit for which the present study is offered as a needed corrective. The dissertation entails a chronological investigation of Jung’s research spanning the period from his seminal 1911-1912 work, Transformations and Symbols of the Libido, to his founding alchemical essays of 1935 and 1936, respectively entitled “Dream Symbols of the Individuation Process” and “Notions of Redemption in Alchemy.” In the first of three sections, Transformations is considered as a template for Jung’s “Dream Symbols” and “Redemption” essays, both in methodology and manner of exposition. Jung’s Red Book is claimed, further, to have shaped the psychological content of those essays, as mediated through published works from the period, 1913 to 1918. The section then chronicles Jung’s final path to the composition of his alchemical essays, as facilitated through an analysis of the quaternary Self symbol, which Jung associated with the historical symbol of the philosophers’ stone. The middle section comprises detailed expositions of Jung’s “Dream Symbols” and “Redemption” essays, as well as commentary upon the materials, means, and methods of his historiography. The last section offers three discrete assessments of Jung’s alchemical thought. It inquires first into the nature of Jung’s historiography, probing the potential shortcomings of his alchemical essays given the historical character and content of the alchemical texts themselves. It also considers Jung’s alchemical findings in light of other identified ‘spiritual-alchemical’ thinkers, in particular, Ethan Allen Hitchcock and Herbert Silberer. Finally, it yields an evaluation of Jung’s alchemical conceptions within the context of his own experiences and writings. Although not supportive of the application of Jung’s findings in the study of Western alchemical history, the dissertation recommends his thought as a creative twentieth-century contribution to such history, framing Jung, himself, as a purveyor of a distinctive ‘psycho-alchemical’ art.