We report a broadband 1H NMR study of the spin dynamics of coated maghemite and gold−maghemite hybrid nanostructures with two different geometries, namely dimers and core−shells. All the samples have a superparamagnetic behavior, displaying a blocking temperature (TB ∼ 80 K (maghemite), ∼105 K (dimer), ∼150 K (core−shell)), and the magnetization reversal time follows the Vogel−Fulcher law. We observed three different anomalies in 1H NMR T1−1 versus T that decrease in amplitude when increasing the applied magnetic field. We suggest that the anomalies are related to three distinct system dynamics: molecular rotations of the organic groups (240 < T < 270 K), superparamagnetic spin blockage (100 < T < 150 K), and surface−core spin dynamics (T < 25 K). By fitting the T1−1 data with a heuristic model, we achieved a good agreement with magnetic relaxation data and literature values for methyl group rotation frequencies.