Rigorous evidence of metallicity of a molecular crystal consisting of single-component neutral molecules is disclosed by observing the Fermi surface through magnetic quantum oscillations. Torque magnetometry measurements of de Haas-van Alphen oscillatory signals in a single crystal of [Ni(tmdt)2] molecules (tmdt = trimethylenetetrathiafulvalenedithiolate) were performed by using a sensitive microcantilever at low temperatures in high magnetic fields to 45 T. The observed signals for all directions of magnetic field revealed unambiguously the presence of three-dimensional Fermi surfaces for both holes and electrons. The results are consistent with electronic band structure calculations for [Ni(tmdt)2].