We show that the ionization of dense molecular clouds can be used to set strong constraints on dark matter models producing UV/X-ray photons in their annihilation or decay. We place robust and competitive constraints on various dark matter models, such as axion-like particles, scalars and sterile neutrinos, for masses between ~eV and ~keV, and project forecasts to illustrate the potential of this target. We discuss how these constraints can be significantly improved by considering a more refined sample of molecular clouds near the Galactic Center and above the Galactic plane, a detailed modeling of the cosmic-ray ionization contribution and, potentially, a more refined analysis of the gas density in clouds through dust extinction maps. Thus, ionization of molecular clouds emerges as one of the most powerful tools for probing sub-keV dark matter.

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