We report what we believe to be the first demonstration of a facile approach with controlled geometry for the production of crystal-core ceramic-clad hybrid fibers for scaling fiber devices to high average powers. The process consists of dip coating a solution of polycrystalline alumina onto a high-crystallinity 40-μm-diameter Ti:sapphire single-crystalline core followed by thermal treatments. Comparison of the measured refractive index with high-resolution transmission electron microscopy reveals that a Ca/Si-rich intragranular layer is precipitated at grain boundaries by impurity segregation and liquid-phase formation due to the relief of misfit strain energy in the Al2O3 matrix, slightly perturbing the refractive index and hence the optical properties. Additionally, electron backscatter diffractions supply further evidence that the Ti:sapphire single-crystalline core provides the template for growth into a sacrificial polycrystalline cladding, bringing the core and cladding into a direct bond. The thus-prepared doped crystal core with the undoped crystal cladding was achieved through the abnormal grain-growth process. The presented results provide a general guideline both for controlling crystal growth and for the performance of hybrid materials and provides insights into how one might design single-mode high-power crystal fiber devices.