This case report describes a pulpotomy treatment of a permanent mature molar tooth with established irreversible pulpitis and condensing apical periodontitis, using calcium-enriched mixture (CEM) cement. Clinical examination revealed that the first right lower molar had a large carious lesion with history of spontaneous/lingering pain; radiographic examination showed condensing apical periodontitis. Pulpotomy was opted as the treatment; cervical pulpotomy was carried out. Following hemostasis, the radicular pulp stumps were covered with ~2-mm-thick layer of the prepared CEM cement; the tooth was restored with amalgam. Two-year follow-up showed that the treated tooth had been symptomless, and there were no clinical signs/symptoms of either inflammation or infection. Radiographically, the periradicular lesion was completely healed with reconstruction of bone structures to normal appearance; the root canals were not calcified. According to chemical, physical, and biological properties of the CEM cement, this novel biomaterial may be suitable for endodontic treatment.