A highly efficient and environmental-benign oxidation by dioxygen (or air) as the sole oxidant was first applied for the conversion of 2-imidazoline-5-carboxylic derivatives to imidazole-5-carboxylic derivatives in very good and excellent yields. The substituent effect on 2-imidazoline ring was investigated. This protocol was also suitable for the synthesis of 2-imidazoles in relatively large scale.