Crystal/glass nanolaminates (NLs) present mutually exclusive mechanical properties by combining the strength of the amorphous phase with the ductility of the crystalline phase. Moreover, reducing the amorphous layer thickness can suppress shear band instability while adjusting the crystalline layer promotes crystal/glass co-deformation, leading to superior strength and plasticity [1]. However, the role of the interface is not well understood. Moreover, BCC/glass NLs remain largely unexplored despite their proven potential to present promote co-deformation due to the difference in the dislocation process of BCC, i.e., screw dislocations moving in multi-planar to cross-slip processes [2]. Here, we present architectural and interface engineering strategies in BCC/glass NLs that effectively suppress shear band instability and promote homogenous co-deformation. 2 µm-thick Fe/Zr40Cu60 NLs were synthesized by magnetron co-sputtering. To investigate the size-dependent shear band instability transition, we varied the Zr40Cu60 thickness (10-90 nm), keeping the Fe at 10 nm. In a second approach, we varied the bilayer period between 20-80 nm at equal volume fractions to investigate the role of the interface density. The hardness (H) and yield strength (σy) of the Fe/Zr40Cu60 NLs exceeds individual layer values, reaching H = 9.6 GPa and σy = 2.14 GPa for the 10/10 nm NLs due to the sharp interfaces blocking the shear band. Micropillar compression tests showed that thicker Zr40Cu60 layers (90 nm) lead to shear band instability, whereas thinner layers show homogenous co-deformation. Combining interface and architecture effects, 20/20 nm NL exhibits an exceptional 45% compressive plasticity and σy = 1.96 GPa. Overall, our findings provide insights into the nanoengineering of crystal/glass NLs by exploiting the interface effects, suppressing shear band instability, and promoting co-deformation effectively. REFERENCES [1] W. Guo et al., Acta Mater, vol. 80, 2014. [2] F. Qin et al., Mater. Sci. Eng. A, vol. 891, 2024.