Rapid, sensitive, and accurate detection of Cr2O72− in the environment is of great significance. This article synthesized water‐soluble N and S‐doped carbon quantum dots (N,S‐CQDs) using a simple hydrothermal self‐assembly pathway through hydrogen bonding of melamine and trithiocyanuric acid. N,S‐CQDs show green fluorescence under visible light excitation at 420 nm, with a high fluorescence quantum yield of 33.4%. Under photo‐induced electron transfer, significant fluorescence dynamic quenching occurred in N,S‐CQDs when a solution containing Cr2O72− was added. Based on this specific response, the selective and sensitive probe for Cr2O72− is achieved, with a wide detection concentration of up to 33 µm. The limits of detection can be as low as 0.11 µm. This work provides an easy‐prepared N,S‐CQDs for sensitive detecting of Cr2O72− in the environment.