The global oil and gas exploration targets are gradually moving towards a new field of oil and gas accumulation with nanopore throats, ranging from millimeter scale to micro-nano pore throats. The development method of tight oil reservoirs is different from that of conventional oil reservoirs, and the development efficiency is constrained. Therefore, it is necessary to construct a nanoscale fluid with strong diffusion and dispersion and improve its permeability, suction, and displacement capabilities. Under the background of CCUS, carbon dioxide flooding is a better way to develop tight reservoirs. However, in order to solve the problem of gas channeling, this paper developed a carbon dioxide-responsive graphene point type surfactant, which has a good gas–liquid synergistic effect. At the same time, graphene nanomaterials are carbon-based and create no environmental damage in oil reservoirs. In this study, graphene quantum dots (GQDs) were prepared using the hydrothermal method, and functional graphene quantum dots (F-GQDs) responsive to carbon dioxide stimulation were synthesized by covalent grafting of amidine functional groups. By characterizing its structure and physical and chemical properties, and by conducting imbibition simulation experiments, its imbibition and drainage ability in nanopore throats is elucidated. Infrared spectrum measurement shows that after functional modification, the quantum dots exhibited new characteristic peaks at 1600 cm−1 to 1300 cm−1, considering the N-H plane-stretching characteristic peak. The fluorescence spectra showed that the fluorescence intensity of F-GQDs was increased after functional modification, which indicated that F-GQDs were successfully synthesized. Through measurements of interfacial activity and adhesion work calculations, the oil–water interfacial tension can achieve ultra-low values within the range of 10−2 to 10−3 mN/m. Oil sand cleaning experiments and indoor simulations of spontaneous imbibition in tight cores demonstrate that F-GQDs exhibit effective oil-washing capabilities and a strong response to carbon dioxide. When combined with carbon dioxide, the system enhances both the rate and efficiency of oil washing. Imbibition recovery can reach more than 50%. The research results provide a certain theoretical basis and data reference for the efficient development of tight reservoirs.