Non-invasive detection based on optical imaging and spectroscopy is an important development direction in the field of biomedical optics. Among which, Raman spectroscopy was widely applied for biomolecular, cellular and bio-tissue level diagnosis due to its advantage of providing biochemical “fingerprint” information of the targets being detected. The detection of thyroid disease, especially the clinical detection of thyroid tumors often involves the combination of multiple methods and techniques, and it faces some degrees of diagnostic challenge, so the development of new detection methods is of great significance. This review mainly focuses on research advances of Raman spectroscopic detection and analysis of single thyroid cells, differentiation and diagnosis between pathological thyroid tissue and normal thyroid tissue (especially our recent research work about silver nanoparticle based surface-enhanced Raman analysis and diagnosis between pathological thyroid tissue and normal thyroid tissue) and recent Raman analysis of thyroid hormones as well. The application prospect and future directions of Raman spectroscopy in this area was also briefly discussed.