Titanium-based materials, which combine high strength and hardness of surface layer along with sufficient ductile characteristics of the matrix metal, are very promising for various applications, particularly, as armoured components in military-industrial complex. Above-mentioned combination of properties can be achieved by means of the creation of multilayer structures, which consist of layers possessing different physical and mechanical properties. In the present study, microstructure peculiarities, mechanical and antiballistic protection properties of the layered Ti-based materials are investigated. Two different ways were used for fabrication of such the layered structures. The first one is a conventional metallurgical (ingot-wrought) method followed by the surface rapid heat treatment of the Ті–6Al–4V and T110 alloys for fabrication of graded structures with different mechanical properties over the material depth. The second one is an elemental powder metallurgy method for fabrication of the structures combining layers of the Ti–6Al–4V alloy and composites based on it and hardened with TiC or TiB particles. Ballistic tests of the obtained materials are carried out for different types of projectiles with different kinetic energy and hardness of the core; features of the penetration of the hitting elements are performed depending on the material structural state. It is proved that materials with graded and layered structures demonstrate undeniable advantages in the antiballistic protection characteristics as compared with homogeneous alloys of the same thickness.