Developing light-driven acid catalyst will be very meaningful for the controlled-acid catalytic processes towards a green chemical industry. Here, based on scanning electrochemical microscopy (SECM) and ΔpH testing, we demonstrate that the 5–10 nm carbon quantum dots (CQDs) synthesized by electrochemical ablation of graphite have strong light-induced proton properties under visible light in solution, which can be used as an acid catalyst. The 5–10 nm CQDs' catalytic activity is strongly dependent on the illumination intensity and the temperature of the reaction system. As an effective visible light driven and controlled acid-catalyst, 5–10 nm CQDs can catalyze a series of organic reactions (esterification, Beckmann rearrangement and aldol condensation) with high conversion (34.7–46.2%, respectively) in water solution under visible light, while the 1–4 nm CQDs and 10–2000 nm graphite do not have such excellent catalytic activity. The use of 5–10 nm CQDs as a light responsive and controllable photocatalyst is truly a novel application of carbon-based nanomaterials, which may significantly push research in the current catalytic industry, environmental pollution and energy issues.