The treatment of neurological disease, such as epilepsy is rather complicated. Emerging therapies such as surgery, gene therapy, stem cell transplantation, and neurostimulation have been developed to replace traditional drug therapy. However, great challenges such as the difficult localization of epileptic foci (EF), incomplete excision of lesioned nerves, high drug resistance, and severe side effects limit their clinical applications. As an alternative, bioinorganic materials have been emerged and show great potentials for epilepsy theranostics. Their unique physical properties, including fluorescence, magnetic resonance effect, and surface‐enhanced Raman scattering effect (SERS), give them the ability to image the localization of EF. In addition, the fluorescence and conductivity of bioinorganic materials could be further used for studying pathogenesis. Moreover, bioinorganic materials could serve as intelligent systems to deliver drugs and cooperative therapy for epilepsy. Herein, this review highlights the design and application of bioinorganic materials in the imaging, diagnosis, and therapy of epilepsy. Furthermore, light is shown on the potential bottlenecks and future perspectives of bioinorganic materials in epilepsy theranostics.