Radiotherapy of head and neck cancer has become more successful with the advances in treatment modalities and use of a multidisciplinary approach. Higher quality treatment and a team approach to radiotherapy have thus been required for head and neck cancer. This study presents the clinical experience of high-dose-rate (HDR) brachytherapy for head and neck cancer treated by a customized intraoral mold technique. Two patients are reported for whom we created dental prostheses as the radiation carriers for HDR brachytherapy of their head and neck cancers. HDR brachytherapy with the dental prostheses reported here was feasible and effective for eradicating the head and neck cancer. It has been demonstrated that HDR brachytherapy using a customized intraoral technique can be a treatment option for patients who are not candidates for surgery or external irradiation. It is strongly suggested that specialized dentists are needed who are familiar with not only the anatomy and function of the head and neck region but also radiotherapy. Dental radiologists should take responsibility for constructing irradiation prostheses. If they do, they have the potential to improve the quality of life of patients who undergo radiotherapy for head and neck cancer.