Metallic glasses, with their short-range order structure, exhibit unique characteristics that do not exist in the corresponding crystalline alloys with the same compositions. These unusual properties are attributed to the absence of translational periodicity, grain boundaries, and compositional homogeneity. Cobalt (Co)-based metallic glassy alloys have been receiving great attention due to their superior mechanical and magnetic properties. Unluckily, Co-Ti alloys and its based alloys are difficult to be prepared in glassy form, due to their rather poor glass-forming ability. In the present work, the mechanical alloying approach was employed to investigate the possibility of preparing homogeneous (Co75Ti25)100−xBx starting from elemental powders. The feedstock materials with the desired compositions were high-energy ball-milled under argon atmosphere for 50 h. The end products of the powders obtained after milling revealed a short-range order structure with a broad amorphization range (2 at% ≤ B ≤ 25 at%). The behaviors of these glassy systems, characterized by the supercooled liquid region, and reduced glass transition temperature, were improved upon increasing B molar fraction. The results had shown that when B content increased, the saturation magnetization was increased, where coercivity was decreased.