The flavoring agent natural vanilla contains an abundant amount of the 4-hydroxy-3-methoxybenzaldehyde (Vanillin) biophenol compound. It is imperative to construct affordable and cost-effective approaches for determining the quantitative composition of Vanillin. In this work, we demonstrate a selective and sensitive electrochemical sensor for the detection of Vanillin by CaMoO 4 /P-CNT/GCE. We characterized our prepared nanomaterial using field emission scanning electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscopy, Raman spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The electrochemical performance and analytical capabilities of this electrochemical sensor were evaluated using cyclic voltammetry, differential pulse voltammetry, and amperometry techniques. As a result of the nanocomposite, high conductivity, and high active surface area, the proposed electrochemical sensor has excellent sensitivity (DPV: 1.9718 and amperometry: 1.0947 μA μM −1 cm −2 ), low detection limit (DPV: 0.0017 and it amperometry: 0.00084 μM), high selectivity, and well reproducibility toward detection of Vanillin. In addition, real-sample analysis confirmed the high performance of the sensor developed in the present study.