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Metallic glass matrix composites may have unique mechanical properties and potential for practical applications. Deformation mechanisms governing the structural evolution process of these mixed structures remain poorly understood. In this article, we elucidate the effect of the crystalline second phase on the tension behavior of metallic glass matrix composites by using large-scale atomistic simulations. We identify that the interaction between the crystalline second phase and the local shear bands is dominated by the cooperative activation of lattice dislocations on the glass–crystal interfaces and discrete shearing events in the neighboring glass matrix. By tailoring the morphology of the crystalline second phase, one observes deflection, bifurcation and suppression of local shear bands and succeeds in enhancing the global plasticity of the composite structure. Guiding principles aimed at designing effective …