We have examined the microstructural evolution of a two-phase composite (olivine + Fe-Ni-S) during large shear deformation, using a newly developed high-pressure X-ray tomography microscope. Two samples were examined: a load-bearing framework–type texture, where the alloy phase (Fe-Ni-S) was present as isolated spherical inclusions, and an interconnected network–type texture, where the alloy phase was concentrated along the silicate grain boundaries and tended to form an interconnected network. The samples, both containing ∼10 vol% alloy inclusions, were compressed to 6 GPa, followed by shear deformation at temperatures up to 800 K. Shear strains were introduced by twisting the samples at high pressure and high temperature. At each imposed shear strain, samples were cooled to ambient temperature and tomographic images collected. The three-dimensional tomographic images were analyzed for textural evolution. We found that in both samples, Fe-Ni-S, which is the weaker phase in the composite, underwent significant deformation. The resulting lens-shaped alloy phase is subparallel to the shear plane and has a laminated, highly anisotropic interconnected weak layer texture. Scanning electron microscopy showed that many alloy inclusions became film-like, with thicknesses <1 μm, suggesting that Fe-Ni-S was highly mobile under nonhydrostatic stress, migrated into silicate grain boundaries, and propagated in a manner similar to melt inclusions in a deforming solid matrix. The grain size of the silicate matrix was significantly reduced under large strain deformation. The strong shape-preferred orientation thus developed can profoundly influence a composite's bulk elastic and rheological properties. High-pressure–high temperature tomography not only provides quantitative observations on textural evolution, but also can be compared with simulation results to derive more rigorous models of the mechanical properties of composite materials relevant to Earth's deep mantle.