The mobility of NH 3 -solvated Cu ions within the zeolite framework has been recently identified as a key factor for the kinetics of the selective catalytic reduction of NO x with NH 3 (NH 3 -SCR) over Cu-zeolite catalysts at low temperatures. Here, we utilize in situ impedance spectroscopy to explore the mobility of NH 3 -solvated Cu II ions, i.e., Cu II (NH 3 ) n , in Cu-SSZ-13 and Cu-ZSM-5 zeolites with varied Cu ion exchange levels, and observed that both the zeolite framework (CHA or MFI) and the Cu exchange level influence the high-frequency dielectric relaxation processes that are associated with the short-range (local) motion of Cu II (NH 3 ) n . Our results suggest that the local motion of Cu II (NH 3 ) n species is favored within the CHA framework due to the unique cage structure, and thereby contribute to the overall ion conductivity at high frequencies, which, on the contrary, is not observed for ZSM-5, where NH 3 -solvated Cu 2+ ions do not experience a comparable constrained space for local motion. This study sheds new light on the mobility of Cu active sites under NH 3 -SCR related reaction conditions and may contribute to an advanced understanding of the underlying mechanism.