This work demonstrates the fabrication of a carbon paste electrode containing NiO/CNTs modified with 1-methyl-3-butylimidazolium bromide as the binder (CPE/1-M-3BIBr/NiO/CNTs), and its applications related to the highly sensitive detection of carmoisine. The CPE/1-M-3BIBr/NiO/CNTs system was successfully utilized for the nanomolar determination of carmoisine at pH = 7.0. The CPE/1-M-3BIBr/NiO/CNTs successfully resolved the oxidation signals of carmoisine and tartrazine with a peak separation of 450 mV. This is the first time that an application of an electrochemical sensor for the simultaneous determination of carmoisine and tartrazine, two important azo dyes, has been reported. In addition, wide dynamic linear concentration ranges (70–650 μM for carmoisine and 0.1–750 μM for tartrazine), low detection limits (20 nM for carmoisine and 0.06 μM tartrazine) and excellent reproducibility were reported. The CPE/1-M-3BIBr/NiO/CNTs were successfully used for the analysis of carmoisine and tartrazine in dried fruit and soft drink samples. © 2017, Springer Science+Business Media, LLC.