Honey adulteration is a major issue in food production, which may reduce the effective components in honey and have a detrimental effect on human health. Herein, laser-induced breakdown spectroscopy (LIBS) combined with chemometric methods was used to fast quantify the adulterant content. Two common types of adulteration, including mixing acacia honey with high fructose corn syrup (HFCS) and rape honey, were quantified with univariate analysis and partial least squares regression (PLSR). In addition, the variable importance was tested with univariable analysis and feature selection methods (genetic algorithm (GA), variable importance in projection (VIP), selectivity ratio (SR)). The results indicated that emissions from Mg II 279.58, 280.30 nm, Mg I 285.25 nm, Ca II 393.37, 396.89 nm, Ca I 422.70 nm, Na I 589.03, 589.64 nm, and K I 766.57, 769.97 nm had compact relationship with adulterant content. Best models for detecting the adulteration ratio of HFCS 55, HFCS 90, and rape honey were achieved by SR-PLSR, VIP-PLSR, and VIP-PLSR, with root-mean-square error (RMSE) of 8.9%, 8.2%, and 4.8%, respectively. This study provided a fast and simple approach for detecting honey adulteration.