A few cases of Graves’ disease after inactivated or messenger RNA(mRNA) vaccine had been reported. However, new onset of Graves’ disease with thyroid storm after adenovirus-vectored vaccination had not been reported in the literature. We de-scribed a case of newly onset of Graves’s disease with thyroid storm after adenovi-rus-vectored coronavirus disease 2019(COVID-19) vaccination (Vaxzevria) 6 days later. Thyroid storm was diagnosed based on thyrotoxicosis and clinical manifestations. Positive anti-thyroid-stimulating hormone receptor antibody, higher titer of thyroid-stimulating immunoglobulin and thyroid ultrasound competitive with the di-agnosis of Graves’ disease. How adenovirus-vectored COVID-19 vaccine can induce Graves’ disease remained unanswered. The excipient with polysorbate 80 of adenovi-rus-vectored COVID-19 vaccine may act as the key which induced Graves’ disease on top of our patient’s genetic background of hyperthyroidism. To our knowledge, this is the first case of Graves’ disease with thyroid storm secondary to adenovirus-vectored COVID-19 vaccine.