Recent investigations have demonstrated that the plasticity of bulk metallic glasses (BMGs) at room temperature can be improved by artificially introducing both macroscopic and microscopic defects. In this work, both surface grooves and multiple shear bands (MLSBs) are concurrently introduced into the surface of a Zr65Cu15Ni10Al10 BMG employing an ultrasonic bonding machine, whose sizes are also tailored by tuning gas pressures and times. After surface treatment, MLSBs appear around grooves due to the pre-plastic deformation, while numerous nano-scale crystals resulting from thermal-induced nanocrystallization appear within the grooves, leading to the emergence of hierarchical structural heterogeneities. As a result, the strength and plasticity are effectively enhanced compared to as-cast samples when suitable experimental parameters are adopted. The plastic deformation mechanisms change from single main shear banding to multiple shear banding. Therefore, the serrated plastic behaviors exhibit a transition from chaotic to self-organized critical dynamics after surface treatment, confirming the modification of the shear banding instability. The present study provides a viable method to tailor the mechanical properties of BMGs and sheds light on their dynamic plastic deformation behaviors.