The successful embedding of different amounts and types of hydrophobic rare earth clusters (Ln = Y, Pr, Eu, Sm, Nd) in various polymer matrices via miniemulsion polymerization is presented. The resulting cluster‐polymer hybrid nanoparticles are spherical in shape and possess a narrow size distribution, as investigated by photon cross correlation spectroscopy (PCCS) and transmission electron microscopy (TEM). The exact Ln‐content in the nanoparticles is exemplarily investigated for Eu‐ and Nd‐containing polymer dispersions via inductively coupled plasma‐optical emission spectrometry (ICP‐OES). As a result of encapsulation more than 1000 mg · L−1 of the hydrophobic Ln‐cluster are successfully dispersed in water. The photophysical properties of the emulsion show the successful avoidance of water from the vicinity of the clusters. Furthermore, a very efficient energy transfer from the ligand and polymeric unit to Eu3+ ions can be observed in dispersion. Based on the different glass transition temperatures (Tg) of the applied polymers, monolayers of the nanoparticles and efficient luminescent thin polymer films are obtained by spin coating. magnified image