Three new dimeric imidazole alkaloids with a methylene bridge, camellimidazole A–C (1–3), were isolated from Keemum black tea. Their structures were completely elucidated by a combination of diverse spectroscopic and single-crystal X-ray diffraction analyses. The plausible formation pathway of camellimidazole A–C was proposed. Compounds 1 and 2 exhibited remarkable protection against H2O2-induced neuronal damage at the concentration of 1.0 μM.