Objective To evaluate the 131I treatment effect in middle and older-aged patients with Graves’ hyperthyroidism. Methods Retrospective analysis was carried out to evaluate that fine and individual 131I treatment effects on the senile Graves hyperthyroidism in 167 cases of middle and older-aged patients. Based on the thyroid size, texture, age, course, antithyroid drugs (ATD) treatment, complication, operation and effective half-life of patients, the individual treatment correction coefficient was introduced to correctly adjust the dose of 131I. The one-year follow-up after treatment was followed. The recurrence of symptoms, side-effects, improvement of thyroid function were used to evaluate the curable effects. Results The clinical symptoms in 167 cases of senile Graves hyperthyroidism patients were significantly improved with fine individual 131I treatment after 3, 6 and 12 months. The serum levels of FT3, FT4 and TSH in patients after treatment were significantly lower than that of pre-treatment (P < 0.05). The complete recovery rate of hyperthyroidism was 80.24% and partial recovery rate of that was 7.78% with total effective rate 98.8%, including 15 cases of thyroid hypofunction (9.0%). Graves ophthalmopathy and hyperthyroidism heart disease were decreased to the rate of 83.72% and 82.14%, respectively. Conclusion Fine individual 131I treatment for middle and older-aged patients with Graves’ hyperthyroidism has good curative effect, and is worth popularization in clinical treatment.