The synthesis of advanced thin film metallic glasses (TFMGs) with tailored composition and engineered microstructures capable to provide a large combination of mutually exclusive mechanical properties (i.e. high strength and ductility) mitigating the shear band (SB) instability, is an open research topic. Here, I will present recent results involving two (2) strategies to finely to improve the mechanical behaviour of TFMGs including (i) the addition of intrinsically ductile elements (Al) and the (ii) development of fully amorphous nanolaminated structures. Firstly, I will provide a holistic picture about the relationship between atomic structure, mechanical properties, and thermal stability of ZrCuAlx TFMGs varying the Al content from 0 to 12 at.%, carrying out a broad characterization involving experiments and ab initio molecular dynamic simulations (AIMD). I will show that the addition of Al resulted in a change of average interatomic distances by ∼10 pm with the formation of shorter bonds (Al-Zr and Al-Cu), influencing the mechanical response (shear/elastic moduli and hardness) which increases by ∼15% for 12 at.% Al. Tensile tests on polymer substrate revealed a maximum value for the crack initiation strain of 2.1% for ZrCuAl9, while the strain-to-failure rapidly decreases at higher Al contents. The observed reduction in damage tolerance is correlated to a transition in atomic configuration. Specifically, a maximum in density of full and defective icosahedral cluster population is observed at 9 at.% Al, inducing a more shear-resistant behavior to the material [1]. Then, I will discuss the fabrication of ZrCu/ZrCuAl9 nanolaminates with different nanoscale bilayer period (Λ, from 200 down to 50 nm). I will show the combined effect of local chemistry variation and nanointerface density influences the propagation of SBs with enhanced plastic deformation (> 10 %) is observed for Λ = 100 and 200 nm during micropillar compression, but accompanied by a reduction of the yield strength. In contrast, for Λ = 50 nm, deformation is dominated by catastrophic SB events, while the yield strength returns to that of the monolithic films of ∼2–2.5 GPa [2]. Overall, I will provide guidelines to the design of compositional and microstructural-tailored TFMGs with tuned mechanical properties with potential for applications. REFERENCES [1] C. Poltronieri … M. Ghidelli, Acta Mater., 258, 119226, 2023. [2] C. Poltronieri … M. Ghidelli, Scripta Mater., 259, 116571, 2025.