Thin film metallic glasses (TFMGs) are emerging materials characterized by outstanding combination of mechanical/electrical properties involving a yield strength close to the theoretical limit, large ductility (> 10%) [1] and metallic-like conductivity [2]. Nevertheless, the synthesis of advanced TFMGs with engineered microstructure and the understanding of their mechanical/electrical properties is barely tackled, requiring the development of novel synthesis strategies and cutting-edge techniques for submicrometer scale characterization. Here, we report the use of Pulsed Laser Deposition (PLD) as a novel technique to synthetize nanostructured Zr50Cu50 (%at.) TFMGs. We show how the control of PLD process parameters (background gas pressure and laser fluence) enables to synthetize different film microstructures involving atom-by-atom or cluster-assembled growth, resulting in a variety of film structures including compact fully amorphous, amorphous nano-porous with large free volume interfaces, and amorphous embedded with nanocrystals. High-resolution TEM reveals a nano-laminated atomic structure characterized by alternated layers with different chemical enrichment and local atomic order. This self-assembled nanoarchitecture is at the basis of unique mechanical properties including large elastic modulus (145 GPa) and hardness (10 GPa). Quantitative in-situ TEM tensile tests reveal that films have an outstanding yield strength (3 GPa) and ductility (> 9%) product which is significantly dependent on the microstructure with large/low plasticity and low/high yield strength obtained for nanogranular/compact metallic glass films. Finally, we 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. [1] M. Ghidelli, H. Idrissi, S. Gravier, J.-J. Blandin, J.-P. Raskin, D. Schryvers, T. Pardoen, Acta Mater. 2017, 131, 246-259. [2] B. Wan An, E.-J. Gwak, K. Kim, Y.-C. Kim, J. Jang, J.-Y. Kim, J.-U. Park, Nano Lett. 2016, 16, 1, 471-478.