Recently, there has been interest in semimetallic rare earth monopnictide nanoparticles epitaxially embedded in III-V semiconductors due to the drastic changes brought about in these materials’ electrical and thermal properties. The properties of terbium codeposited with gallium arsenide by molecular beam epitaxy are discussed here. These new materials were characterized by x-ray diffraction, Rutherford backscattering spectrometry, resistivity measurements, photoluminescence, time-domain thermoreflectance thermal conductivity measurements, optical absorption spectroscopy, and plan-view high-angle annular dark-field scanning transmission electron microscopy. Results revealed successful formation of randomly distributed nanoparticles with an average diameter of ∼1.5 nm, reduction of thermal conductivity by a factor of about 5, and consistency with theoretical predictions of mid-band-gap Fermi level pinning and behavior of past similar materials. The success of these TbAs:GaAs materials will lead the way for growth of similar materials [TbAs:InGa(Al)As] which are expected to exhibit highly desirable thermoelectric properties.