The synthesis of advanced thin film metallic glasses (TFMGs) with engineered microstructures capable to provide a large combination of mutually exclusive mechanical properties (i.e. high strength and ductility) is an open research topic. Here, I will present recent results involving two (2) strategies to finely tune the microstructure of TFMGs down to the atomic scale, resulting in outstanding and controlled mechanical behavior. Firstly, I will show the potential of Pulsed Laser Deposition (PLD) as a novel technique to synthetize nanostructured Zr50Cu50 (%at.) TFMGs. Specifically, a variety of TFMG microstructures – among which amorphous nanogranular films showing large free volume interfaces and a nanolaminated self-assembled atomic structures – have been deposited. This results in an unique mechanical behavior as shown by in situ TEM/SEM tensile/compression tests, reporting homogeneous deformation combined with a large yield strength (>3 GPa) and ductility (>9 %) product [1]. Then, I will focus on the fabrication of fully amorphous nanolaminates with nanoscale period. I will show how the control of the sublayer thickness (from 100 down to 5 nm) influences the deformation behavior, while tuning the mechanical properties. Specifically, fully amorphous (Zr24Cu76/Zr61Cu39 %at.) nanolaminates with bilayer period <50 nm limit shear band/crack propagation, while providing a good combination of large ductility (> 10%) and yield strength (>1.5 GPa). Overall, our results pave the way to the development of novel TFMGs with improved mechanical properties and wide application range. [1] M. Ghidelli et al., Acta Mater., 213, 116955, 2021.