AbstractHere, a rational strategy to achieve multifunctional N, S codoped carbon dots (N, S‐CDs) is reported, aiming to improve the photoluminescence quantum yields (PLQYs) of the CDs. The synthesized N, S‐CDs have excellent stability and emission properties independent of excitation wavelength. Through the introduction of S element doping, the fluorescence emission of CDs is red‐shifted from 430 to 545 nm, and the corresponding PLQYs can be greatly enhanced from 11.2% to 65.1%. It is found that the doping of S elements causes an increase in the size of CDs and an elevated graphite N content, which may be the key factors to cause the redshift of fluorescence emission. Furthermore, the introduction of S element also serves to suppress the nonradiative transitions, which may be responsible for the elevated PLQYs. Besides, the synthesized N, S‐CDs have certain solvent effect and can be applied to detect water content in organic solvents, and have strong sensitivity to alkaline environment. More importantly, the N, S‐CDs can be used to achieve an “on–off–on” dual detection mode between Zr⁴⁺ and NO₂⁻. In addition, N, S‐CDs combinedwith polyvinylpyrrolidone (PVP) can also be utilized as fluorescent inks for anti‐counterfeiting applications.