Multifunctional materials with more than two good properties are widely required in modern industries. However, some properties are often trade-off with each other by single microstructural designation. For example, nanostructured materials have high strength, but low ductility and thermal stability. Here by means of spark plasma sintering (SPS) of nitrided Ti particles, we synthesized bulk core-shell structured Ti alloys with isolated soft coarse-grained Ti cores and hard Ti-N solid solution shells. The core-shell Ti alloys exhibit a high yield strength (~1.4 GPa) comparable to that of nanostructured states and high thermal stability (over 1100 °C, 0.71 of melting temperature), contributed by the hard Ti-N shells, as well as a good plasticity (fracture plasticity of 12%) due to the soft Ti cores. Our results demonstrate that this core-shell structure offers a design pathway towards an advanced material with enhancing strength-plasticity-thermal stability synergy.