Carbon-based nanoparticles possess ultrasmall size (<10 nm) and show great application potential in reducing the injection pressure of unconventional reservoirs. However, the strong hydrophilicity of carbon nanoparticles limits the oil−water interfacial activity, which hinders the further improvement of oil recovery. In this study, active carbon dots (S-CDs) are synthesized through two-step hydrothermal reactions by first preparing carbon dot (CD) carriers from citric acid and ethylenediamine and then grafting cocamidopropyl-N,N-dimethylglycine and characterizing them by high-resolution transmission electron microscopy, atomic force microscopy, Fourier transform infrared spectroscopy, and Xray photoelectron spectroscopy. The stability experiment verifies that the abundant hydrophilic groups on the surface substantially enhance the electrostatic repulsion between S-CDs, and the absence of carboxyl groups avoids the reaction with other groups, which endows S-CDs with intrinsic aqueous dispersibility and resistance to high temperature (130 °C) and high salinity (16 × 10 4 mg/L). In addition, S-CDs with an average hydration particle size of 2.84 nm exhibit excellent oil−water and oil−solid interfacial activity by controlling the interfacial tension, interfacial viscoelastic modulus, wettability alteration, and adsorption capacity. Core flooding tests show that 0.05 wt % S-CD nanofluids can reduce the injection pressure by 32.92% and increase the oil recovery rate by 19.15% compared to simulated formation water.