The quantum yield and fluorescence properties of carbon dots are key issues for environmental detection. In this study, nitrogen–sulfur-doped carbon dots (N,S-CDs) were prepared hydrothermally by adding thiourea to provide the N source. By adjusting the ratio of citric acid (CA) to thiourea (N,S) and adding anhydrous ethanol, blue fluorescent doped carbon dots with a quantum yield of up to 53.80% were obtained. The particle morphology and crystalline organization of the N,S-CDs were analyzed using transmission electron microscopy (TEM) and X-ray diffraction (XRD). Fourier transform infrared (FTIR) spectroscopy was used to illuminate distinct functional units through the recording of typical vibration bands. The luminescence properties of the N,S-CDs were investigated using ultraviolet–visible (UV-vis) absorption spectroscopy and steady-state fluorescence spectroscopy (PL). In addition, the fluorescence stability of the N,S-CDs was studied in detail. The results showed that the functional groups of the N,S-CDs chelate Fe3+ ions to quench the fluorescence of carbon dots. This shows that the N,S-CDs exhibit high selectivity for Fe3+ ions. With the addition of Fe3+ in the concentration of 0–100 µM, the fluorescence intensity of the N,S-CDs exhibited distinct and linear dependence upon the Fe3+ concentration (R2 = 0.9965), and the detection limit (D = 3ơ/m) was measured as 0.2 µM. The excellent optical properties and Fe3+ selectivity of the N,S-CDs provide a huge boost for application in the field of environmental monitoring.