Graphitic carbon nitride (g-C3N4) has received much interest as a visible-light-driven photocatalyst for degrading pollutants such as organic dyes and antibiotics. However, g-C3N4 bulk activity could not meet expectations due to its rapid recombination of photogenerated electron–hole pairs and low specific surface area. In our study, melamine was thermally treated one-step in the presence of NH4Cl to produce g-C3N4 nanosheets. The characterizations of surface morphology and optical properties of all g-C3N4 samples were investigated by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectrum (XPS), transmission electron microscopy (TEM), and UV–visible diffuse reflectance spectroscopy. Compared to bulk g-C3N4, g-C3N4 nanosheets demonstrated excellent photocatalytic activities, with approximately 98% RhB removal after 210 min of visible light irradiation. Furthermore, the effect of catalyst dosage, pH, and RhB concentration on the removal percentage dye of g-C3N4 nanosheets was also investigated. h+ and •O2− species were demonstrated as the key reactive species for the RhB. Besides, ECN exposed a tetracycline degradation efficiency of 80.5% under visible-light irradiation for 210 min, which is higher than BCN (60.8%). The improved photocatalytic activity of g-C3N4 nanosheets is due to the restriction of the recombination of photogenerated electrons/hole pairs, as provided by photoluminescence spectra and Nyquist plot. As a result, our research may offer an effective approach to fabricating g-C3N4 nanosheets with high photocatalytic activity and high stability for environmental decontamination.