Zearalenone (ZEN) is a contaminant found naturally in grains such as wheat that poses a potential threat to human and animal health. This study describes a colorimetric sensor array detection system based on chemically reactive dyes and chemometric algorithms for the determination of ZEN in wheat. Firstly, six chemically responsive dyes were screened to construct a colorimetric sensor array to obtain the response fingerprints of the volatile components of wheat. The RGB differences of the chemically reactive dyes before and after the response were then calculated to obtain the color component data of the image. The maximum information coefficient (MIC) and ReliefF methods were then used to select the best color features. Finally, the Support Vector Machine Regression (SVR) prediction model was developed and validated based on the optimized features on 132 sample sets. The results showed that the SVR model developed on the initial 132 wheat samples had good predictive ability. Its root mean square error (RMSE) on the prediction set was 38.1625 μg∙kg−1 with a correlation coefficient (R) 0.9516. In particular, the SVR model combining 13 color components reduced the RMSE on the prediction set to 30.4484 μg∙kg−1, with an improved R of 0.9695. Olfactory visualization techniques were shown to be effective for the determination of ZEN in wheat. This study is expected to provide a scientifically novel approach for quality stabilization during the storage of wheat or other cereals.