Abstract Carbon nanodots (C‐dots) show great potential as an important material for biochemical sensing, energy conversion, photocatalysis, and optoelectronics because of their water solubility, chemical inertness, low toxicity, and photo‐ and electronic properties. Numerous methods have been proposed for the preparation of C‐dots. However, complex procedures and strong acid treatments are often required, and the as‐prepared C‐dots tend to be of low quality, and in particular, have a low efficiency for photoluminescence. Herein, a facile and general strategy involving the electrochemical carbonization of low‐molecular‐weight alcohols is proposed. As precursors, the alcohols transited into carbon‐containing particles after electrochemical carbonization under basic conditions. The resultant C‐dots exhibit excellent excitation‐ and size‐dependent fluorescence without the need for complicated purification and passivation procedures. The sizes of the as‐prepared C‐dots can be adjusted by varying the applied potential. High‐quality C‐dots are prepared successfully from different small molecular alcohols, suggesting that this research provides a new, highly universal method for the preparation of fluorescent C‐dots. In addition, luminescence microscopy of the C‐dots is demonstrated in human cancer cells. The results indicate that the as‐prepared C‐dots have low toxicity and can be used in imaging applications.