Tobacco mosaic virus (TMV) has long been exploited as a robust biological scaffold for organic/inorganic modification owing to its anisotropic structure and chemically addressable amino acid residues on both the exterior and interior. We present the fabrication of a crystalline microporous metal-organic framework (MOF) shell on the exterior of TMV, which retains its rod-like morphology, and produces uniformly formed core-shell structures with high accessible surface area and pore volume. We also describe an exfoliation method that can recover the intact viral particle from the core-shell composite.