Edible gelatin has been widely used as a food additive in the food industry, and illegal adulteration with industrial gelatin will cause serious harm to human health. The present work used laser-induced breakdown spectroscopy (LIBS) coupled with the partial least square–support vector machine (PLS-SVM) method for the fast and accurate estimation of edible gelatin adulteration. Gelatin samples with 11 different adulteration ratios were prepared by mixing pure edible gelatin with industrial gelatin, and the LIBS spectra were recorded to analyze their elemental composition differences. The PLS, SVM, and PLS-SVM models were separately built for the prediction of gelatin adulteration ratios, and the hybrid PLS-SVM model yielded a better performance than only the PLS and SVM models. Besides, four different variable selection methods, including competitive adaptive reweighted sampling (CARS), Monte Carlo uninformative variable elimination (MC-UVE), random frog (RF), and principal component analysis (PCA), were adopted to combine with the SVM model for comparative study; the results further demonstrated that the PLS-SVM model was superior to the other SVM models. This study reveals that the hybrid PLS-SVM model, with the advantages of low computational time and high prediction accuracy, can be employed as a preferred method for the accurate estimation of edible gelatin adulteration.