Electrochemical sensors, particularly those based on ion transfer at the interface between two immiscible electrolyte solutions (ITIES), offer significant advantages such as high selectivity, ease of fabrication, and cost effectiveness for toxic metal ion detection. However, distinguishing between cyclic voltammograms (CVs) of analytes with closely spaced half-wave potentials, such as Cd²⁺ and Cu²⁺, remains a challenge, especially for non-expert users. In this work, we present a novel methodology that integrates advanced artificial intelligence (AI) models with ITIES-based sensing to automate and enhance metal ion detection. Our approach first employed a convolutional neural network to classify CVs as either ideal or faulty with an accuracy exceeding 95 percent. Ideal CVs were then further analyzed for metal ion identification, achieving a classification accuracy of 99.15 percent between Cd²⁺ and Cu²⁺ responses. Following classification, an artificial neural network was used to quantitatively predict metal ion concentrations, yielding low mean absolute errors of 0.0158 for Cd²⁺ and 0.0127 for Cu²⁺. This integrated AI–ITIES system not only provides a scientific methodology for differentiating analyte responses based on electrochemical signatures but also substantially lowers the expertise barrier for sensor signal interpretation. To our knowledge, this is the first report of the AI-assisted differentiation and quantification of metal ions from ITIES-based CVs, establishing a robust framework for the future development of user-friendly, automated electrochemical sensing platforms for environmental and biological applications.