Thin film metallic glasses (TFMGs) are object of intense research due to their a unique combination of mechanical properties involving large yield strength (~3 GPa) and ductility (>10%) [1]. Nevertheless, the synthesis of advanced TFMGs with engineered microstructure and the understanding of their mechanical properties are barely tackled. Here, I will present recent results involving two (2) strategies to develop nanoengineered TFMGs with a controlled microstructure down to the atomic scale, resulting in outstanding and tunable mechanical properties. In the first case, I will show the potential of Pulsed Laser Deposition (PLD) as a novel technique to synthetize nanostructured Zr50Cu50 (%at.) TFMGs. I will show how the control of PLD process parameters enables to synthetize a variety of film microstructures among which compact fully amorphous and amorphous nanogranular, showing lower density and large free volume interfaces [2]. High-resolution TEM reveals a nano-laminated self-assembled atomic structure characterized by alternated layers with different chemical enrichment [2]. This results in an unique mechanical behavior as shown by in situ TEM/SEM tensile/compression tests, reporting homogeneous deformation for nanogranular (cluster assembled) TFMGs in combination with a large yield strength (>3 GPa) and ductility (>9 %) [2]. In the second case, I will focus on the fabrication of multilayers with nanoscale period alternating either fully amorphous or amorphous/crystalline sublayers. I will show how the control of the sublayer thickness (form 100 down to 5 nm) influences the deformation behavior affecting shear bands formation, while tuning the mechanical properties. As an example, alternating CrCoNi (crystalline)/TiZrNbHf (amorphous) nanolayers results in an ultrahigh compressive yield strength (3.6 GPa) and large homogeneous deformation (~15%) [3]. Similarly, I will show the suppression of shear band/crack process in fully amorphous (Zr24Cu76/Zr61Cu39 %at.) multilayers with bilayer period < 50 nm, while keeping a mutual combination of large ductility (> 10%) and yields strength (>2.5 GPa). Overall, our results pave the way to the development of novel amorphous materials with improved mechanical properties and wide application range especially in the field of microelectronics. References: [1] M. Ghidelli et al. Acta Mater., 131, 246, 2017. [2] M. Ghidelli et al. Acta Mater., 213, 116955, 2021. [3] G. Wu et al., Materials Today, 51, 6, 2021.