In the present work, irregular Cu nanoparticle-decorated boron−carbon−nitrogen (Cu−BCN) nanosheets were successfully synthesized. A Cu−BCN dispersion was deposited on a bare glassy carbon electrode (GCE) to prepare an electrochemical sensor (Cu−BCN/GCE) for the detection of chloramphenicol (CAP) in the environment. Cu−BCN was characterized using high-resolution scanning transmission electron microscopy (HRSTEM), scanning electron microscopy (SEM), X-ray diffraction (XRD) analysis, and X-ray photoelectron spectroscopy (XPS). The performance of the Cu−BCN/GCE was studied using electrochemical impedance spectroscopy (EIS), and its advantages were proven by electrode comparison. Differential pulse voltammetry (DPV) was used to optimize the experimental conditions, including the amount of Cu−BCN deposited, enrichment potential, deposition time, and pH of the electrolyte. A linear relationship between the CAP concentration and current response was obtained under the optimized experimental conditions, with a wide linear range and a limit of detection (LOD) of 2.41 nmol/L. Cu−BCN/GCE exhibited high stability, reproducibility, and repeatability. In the presence of various organic and inorganic species, the influence of the Cu−BCN-based sensor on the current response of CAP was less than 5%. Notably, the prepared sensor exhibited excellent performance in real-water samples, with satisfactory recovery.