Univariate and multivariate analyses of strontium (Sr) and vanadium (V) elements in soil have been performed using laser-induced breakdown spectroscopy technology. Thirty-three samples were used as a calibration set, and 11 samples were used as a prediction set. The results demonstrated that the correlation coefficients of the calibration curves method were poor due to the matrix effect. Then, the multivariate models of partial least-squares regression and least squares support vector regression (LS-SVR) were used to construct models. The analysis accuracy was improved effectively by the LS-SVR method, and the correlation coefficient is 0.999 for Sr and 0.983 for V. The average relative errors for the prediction set are lower than 7.45% and 2.88% for Sr and V, respectively. The results indicated that the LIBS technique coupled with LS-SVR could be a reliable and accurate method in the quantitative determination of elemental Sr and V in complex matrices like soil.