/ AbstractWe report on the search for X-ray radiation as predicted from dynamical quantum collapse with low-energy electronic recoil data in the energy range of 1-140 keV from the first science run of the XENONnT dark matter detector. Spontaneous radiation is an unavoidable effect of dynamical collapse models, which were introduced as a possible solution to the long-standing measurement problem in quantum mechanics. The analysis utilizes a model that for the first time accounts for cancellation effects in the emitted spectrum, which arise in the X-ray range due to the opposing electron-proton charges in xenon atoms. New world-leading limits on the free parameters of the Markovian continuous spontaneous localization and Diósi-Penrose models are set, improving previous best constraints by two orders of magnitude and a factor of five, respectively. The original values proposed for the strength and the correlation length of the continuous spontaneous localization model are excluded experimentally for the first time.