Freestanding flexible membranes based on biocompatible calcium phosphates are of great interest in regenerative medicine. Here, the authors report the first synthesis of well-aligned biomimetic hexagonal bars of hydroxyapatite (HAp) on flexible, freestanding mesoporous graphene/single-walled carbon nanotubes (MG/SWCNT) hybrid membranes. The chemical composition and surface morphology of the HAp coating resemble those of biological apatite. Nitrogen doping and oxygen plasma etching of the MG/SWCNT membranes increase the density of nucleation sites and yield more uniform coatings. This novel membrane favors the attachment and proliferation of human fetal osteoblast (hFOB) osteoprogenitor cells. When soaked in simulated body fluid, enhanced in vitro biomineralization occurs on the hybrid membranes. This hybrid membrane holds great promise in biomedical applications such as patches and strips for spine fusion, bone repair, and restoration of tooth enamel.