In this study, the effects of starting material types on graphene oxide (GO) are reported with the aim of developing graphene (GR) synthesis. The GOs were prepared from natural graphite (NG) powder and graphite nanoplate (GNp) based on the Hummers method. Two kinds of GR were successfully synthesized using GOs, which were prepared from NG and GNp in the presence of hydrazine and ammonia for 24 h at a 100 degrees C reaction temperature. The synthesized GOs and GRs were characterized by X-ray diffraction (XRD) techniques, Fourier transform infrared, high-contrast transmission electron microscopy (HCTEM), dispersive Raman spectroscopic analyses, and elemental analyses. HCTEM analyses of GOs and GRs exhibited largely folded, convoluted, and entwined GO and GR structures. The XRD and Raman analyses showed that the number of layers of GO1, GO2, GR1, and GR2 were 9.27, 13.53, 4.11, and 5.26, respectively. On the other hand, GR1, prepared from NG powder, showed much higher quality (peak intensities (I-D/I-G) = 1.53, C/O = 3.64) than GR2, which was prepared from GNp (I-D/I-G = 1.64, C/O = 3.17). Thus, this study provides a way to produce higher quality GOs and GRs.