The role of radiothallium201Tl chloride scintigraphy was evaluated in 117 patients with solitary thyroid nodules, demonstrated as nonfunctioning with99mTc pertechnetate, and in which histologic diagnosis was obtained. The nodules were malignant in 25 patients and benign in 92. In an attempt to improve the initial diagnostic discrimination between malignant and benign lesions, the degree of accumulation of201Tl by the nodule was assessed semiquantiatively. The uptake was graded by comparing the accumulation by the nodule with that in the paranodular tissue (PN) (1‐absent; 2‐minimal uptake but lower than in PN; 3‐uptake equal to PN; 4‐mildly preferential uptake in comparison with PN; 5‐markedly increased uptake). None of the patients with grade 1 or grade 2 uptake had malignant disease. Of 25 patients with histologically confirmed cysts, 21 had uptake of grade 1 and 4 of grade 2. Benign adenomas (67 patients) were associated with all grades, 45% having grade 3 uptake. Uptake of201Tl in malignant lesions was in all instances at least equal to paranodular tissue or higher (grades 3–5). The incidence of malignancy was 17% in grade 3, 15% in grade 4, and 67% in grade 5 uptake. It is considered that thallium scintigraphy is not by itself a definitive investigation for thyroid cancer but, since the predictive value of malignancy with strict decision threshold (grades 1–4 considered normal and grade 5 abnormal) is 67%, and predictive value of a negative test is 90%, the procedure does have a useful role in investigation of nonfunctioning solitary thyroid nodules either by heightening the suspicion of malignancy or by indicating a very low probability of malignant change.