Thin film metallic glasses (TFMGs) are emerging materials characterized by a unique combination of mechanical/electrical properties involving large yield strength close to the theoretical limit, large ductility (> 10%) and metallic-like electrical conductivity. Nevertheless, the synthesis of advanced TFMGs with engineered microstructure as well as the understanding of their mechanical properties are barely tackled, limiting potential applications. 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/functional properties. In the first case, the potential of Pulsed Laser Deposition (PLD) as a novel technique to synthetize nanostructured Zr50Cu50 (%at.) TFMGs will be presented. 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 (Fig. a) [1]. High-resolution TEM reveals a nano-laminated self-assembled atomic structure characterized by alternated layers with different chemical enrichment, resulting in unique mechanical properties as shown by in-situ TEM tensile tests reporting a tunable yield strength (>3 GPa) and ductility (> 9%) (Fig. a) [1]. We exploit these properties to developed a stretchable transparent electrode based on nanogranular TFMGs nanotrough network showing excellent stretchability (70%) and low sheet resistance (~3 Ω/sq) which is then integrated in wirelessly rechargeable transparent heater, demonstrating the potential of these films for novel stretchable electronic devices [2]. In the second case, we develop a crystal-glass multilayer system alternating CrCoNi (crystalline)/TiZrNbHf (amorphous) nanolayers (Fig. b) [3]. This system show an ultrahigh compressive yield strength of 3.6 GPa and large homogeneous deformation of ~15% strain surpassing those of conventional TFMGs and nanolaminate alloys (Fig. b). Furthermore, the alloy exhibits ~200 K higher crystallization temperature (Tx> 973 K) compared to that of the original TiZrNbHf-based amorphous phase. The elemental partitioning among adjacent amorphous and crystalline phases leads to their mutual thermodynamic and mechanical stabilization, opening up a new symbiotic approach for stable, strong and ductile materials [3]. References [1] M. Ghidelli et al. Acta Materialia 213 (2021), 116955 [2] S. Lee et al., Nano Letters, 20, (2020), 4872–4881. [3] G. Wu et al., Symbiotic crystal-glass alloys via dynamic chemical partitioning, Materials Today (2021), in-press.