In this study, an iterative method using polarized Raman spectroscopy to quantitatively determine all the in-plane components of the stress tensor in semiconductor structures is presented. Raman experiments were conducted on silicon at different stress states. The results obtained by the proposed method were in good agreement with the given stress state. In addition, the effect of random errors of Raman shifts on the stress component calculation is discussed. In contrast to the conventional analytical solution, our iterative method can significantly reduce the random errors.