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Disordered superconducting nitrides with kinetic inductance have long been considered to be leading material candidates for high‐inductance quantum‐circuit applications. Despite continuing efforts toward reducing material dimensions to increase the kinetic inductance and the corresponding circuit impedance, achieving further improvements without compromising material quality has become a fundamental challenge. To this end, a method to drastically increase the kinetic inductance of superconducting materials via spinodal decomposition while maintaining a low microwave loss is proposed. Epitaxial Ti0.48Al0.52N is used as a model system and the utilization of spinodal decomposition to trigger the insulator‐to‐superconductor transition with a drastically enhanced material disorder is demonstrated. The measured kinetic inductance increases by two to three orders of magnitude compared with the best disordered superconducting nitrides reported to date. This work paves the way for substantially enhancing and deterministically controlling the inductance for advanced superconducting quantum circuits.