We report magnetoelectric coupling in nanoparticle assemblies that persists to temperatures over 300 times lower than in previous studies. The ME response saturates at low temperature, revealing a quantum plateau of the coupling. A field dependence analysis shows a crossover from quadratic to linear behavior, captured by a phenomenological expansion . The magnitude of the extracted quadratic coefficient, , follows a power law with , indicating proximity to a quantum critical regime. The observed saturation reflects a new intrinsic energy scale, distinct from finite-size or extrinsic effects. These results establish nanoparticle assemblies as a new platform for studying quantum magnetoelectric phenomena.

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