Shear banding behavior of metallic glasses (MGs) strongly correlates with the microstructural heterogeneity. Understanding how the nucleation and propagation of shear bands are governed by the nanoscale structural heterogeneity is crucial for designing high-performance MGs. Herein, the traditional molecular dynamics (MD) and swap Monte Carlo (SMC) simulations are used to construct two phases of CuZr metallic glasses: the soft phase with a high cooling rate about 10¹³ K/s, and the hard phase with a extremely low cooling rate in simulations about 10⁴ K/s. The soft phase contains fewer icosahedral clusters, allowing for easier plastic deformation; the hard phase has more of icosahedral clusters, which promotes shear localization once shear bands form inside. A ductile-to-brittle transition is found to occur in the soft-and-hard phase ordered MGs with the increase of the hard-region fraction c. Additionally, the strategy for ordering these two phases to strongly influence the mechanical behavior of MGs is proposed. Dispersed and isolated hard-regions can improve the mechanical stability of MGs and delay the occurrence of shear banding. Instead, the soft regions surrounded by hard regions can induce a secondary shear band that is formed through the reorientation of plastic zones under constrained deformation, leading to more delocalized plastic deformation zones. This work reveals that the structural heterogeneity achieved by adjusting the topology of soft and hard phases can significantly change the mechanical performance of MGs, which can guide the design of metallic glasses with controllable structures through architectural ordering strategies.