Novel chemical routes to high-quality nanodispersed quantum dots of Zn3P2 have been developed. The precursors Me2Zn and HPtBu2 were thermolyzed in TOPO (tri-n-phosphine oxide) or 4-ethylpyridine, resulting in capped nanomaterial. The nanoparticulates described in this work were capped with either TOPO or 4-ethylpyridine and had optical properties similar to II3−V2 compounds prepared by aqueous routes. The as-prepared nanoparticulates were polydispersed (standard deviation of ca. 20%) and appeared to be a mixture of both crystalline and amorphous materials. The nanoparticles were found show quantum confinement effects with band gaps shifted to much higher energies. Luminescence was strong and exhibited large Stokes shifts relative to the absorption edge, probably due to metal vacancies being efficient trapping sites for charge carriers