In this work, the role of individual B2 particles with bimodal length scale on work-hardening and plastic deformation behaviors of Ti-based bulk metallic glass composites has been studied by systemic microstructural and mechanical investigations. At the early stage of plastic deformation, work-hardening characteristic was clearly observed. This work-hardening behavior can be supported by the martensitic transformation and the deformation induced twinning in both small- and large-sized B2 particles during deformation. On progress of plastic deformation after work-hardening, small-sized B2 particles (1–10 μm) were penetrated by propagation of main shear bands while large-sized B2 particles (100–200 μm) were severely interacted with shear bands leading to formation of multiple shear bands and impeding the propagation of principal shear bands. This reveals that each B2 particle with different length scale plays a distinct role on the stage of plastic deformation depending on the particle size.