A novel multifunctional colorimetric sensor HMBC ((E)‐3‐((2‐hydroxy‐3‐methoxybenzylidene)amino)benzofuran‐2‐carboxamide), based on 3‐aminobenzofuran‐2‐carboxamide and 2‐hydroxyl‐3‐methoxylbenzaldehyde, was designed and synthesized. The chemosensor HMBC could sense Co2+, Cu2+, and Zn2+ by color changes from colorless to yellow. Limits of detection (0.38, 0.41, and 1.02 μM) of HMBC for Co2+, Cu2+, and Zn2+ were much lower than the New Jersey Department of Environmental Protection (NJDEP) standard (1.70 μM) for Co2+ and the WHO guidelines (31.5 μM and 76 μM) for Cu2+ and Zn2+. Significantly, HMBC could be applied for the quantification of Co2+, Cu2+, and Zn2+ in real samples. The sensing process of HMBC for Co2+, Cu2+, and Zn2+ was well demonstrated by 1H NMR and UV–Visible titrations, Job plots, theoretical calculations, and ESI‐mass spectroscopy.