A simple one-step hydrothermal method was developed to synthesize pyrite (FeS2) sheet- and bulklike pyrite mineral. The Fe/S molar ratio determines the phase of FeS2, including pyrite and marcasite. The reaction temperature and time are key factors to regulate the structure, morphology, and size of pyrite. Scanning electron and transmission electron microscopy showed the formation of monodisperse microspherulite within 1 h reaction time, and the particles aggregated to large irregular polyhedron particles with increasing reaction time up to 4 h. Electrochemical oxidation tests demonstrated that their electrochemical activity significantly decreased with increasing synthesis time. At an elevated temperature of 200 °C, bulk pyrite was obtained after a 24 h reaction time, which could have promising applications in hydrothermal pyrite ore oxidation research.