Conventional methods for detecting unsaturated fatty acids (UFAs) pose challenges for rapid analyses due to the need for complex pretreatment and expensive instruments. Here, we developed an intelligent platform for facile and low-cost analysis of UFAs by combining a smartphone-assisted colorimetric sensor array (CSA) based on MnO 2 nanozymes with "image segmentation-feature extraction" deep learning (ISFE-DL). Density functional theory predictions were validated by doping experiments using Ag, Pd, and Pt, which enhanced the catalytic activity of the MnO 2 nanozymes. A CSA mimicking mammalian olfactory system was constructed with the principle that UFAs competitively inhibit the oxidization of the enzyme substrate, resulting in color changes in the nanozyme−ABTS substrate system. Through linear discriminant analysis coupled with the smartphone App "Quick Viewer" that utilizes multihole parallel acquisition technology, oleic acid (OA), linoleic acid (LA), α-linolenic acid (ALA), and their mixtures were clearly discriminated; various edible vegetable oils, different camellia oils (CAO), and adulterated CAOs were also successfully distinguished. Furthermore, the ISFE-DL method was combined in multicomponent quantitative analysis. The sensing elements of the CSA (3 × 4) were individually segmented for single-hole feature extraction containing information from 38,868 images of three UFAs, thereby allowing for the extraction of more features and augmenting sample size. After training with the MobileNetV3 small model, the determination coefficients of OA, LA, and ALA were 0.9969, 0.9668, and 0.7393, respectively. The model was embedded in the smartphone App "Intelligent Analysis Master" for one-click quantification. We provide an innovative approach for intelligent and efficient qualitative and quantitative analysis of UFAs and other compounds with similar characteristics.