The current trend toward miniaturization in devices components in key technologies such as micro-/nanoelectronics, energy production, sensors and wear protection requires the development of high-performance nanostructured films with superior mechanical properties. Especially, mutually excluding structural properties such as high yield strength and ductility need to be combined, but also high adhesion with the substrate and large fatigue resistance. In order to trigger microstructure-induced material properties, control of the micro-scale structure, atomic composition, average grain size, and layer/film thickness must be optimized based on nanoengineering design concepts. Here, I will present recent results for several class of advanced thin film materials including nanostructured metallic glasses (ZrCu/O, ZrCuAl/O…)[1-3] high entropy alloys (CoCuCrFeNi, Al/CoCuCrFeNi) and nanolaminates (fully amorphous, amorphous/crystalline)[4], showing how the control of micro-structure affect the and micro-scale mechanical behavior and enable ultimate mechanical properties. Among the main results, I will show the potential of Pulsed Laser Deposition (PLD)[1, 2] as a novel technique to synthetize nanostructured cluster-assembled ZrCu, ZrCuAl/O, and CoCuCrFeNi films reaching ultimate yield strength (>4 GPa) and ductility (>15 %) for ZrCuAl/O films. I will show how the control of the sublayer thickness (from 100 down to 5 nm) in fully amorphous nanolaminates influences the deformation behavior suppressing the shear bands formation, while tuning the mechanical properties with mutual combination of large ductility (> 10%) and yields strength (>2.5 GPa). Finally, I will show how alternating CrCoNi (crystalline)/TiZrNbHf (amorphous) nanolayers results in an high compressive yield strength (3.6 GPa) and large homogeneous deformation (~15%)[4]. Overall, our results pave the way to the development of nanostructured thin films with boosted mechanical properties and wide application range. References [1] M. Ghidelli et. al., Novel class of nanostructured metallic glass films with superior and tunable mechanical properties, Acta Mater. 213 (2021) 116955. [2] C. Poltronieri et al., Mechanical properties and thermal stability of ZrCuAlx thin film metallic glasses: Experiments and first-principle calculations, Acta Mater. 258 (2023) 119226. [3] A. Brognara, et al., Effect of composition and nanostructure on the mechanical properties and thermal stability of Zr100-xCux thin film metallic glasses, Mater. Design 219 (2022) 110752. [4] G. Wu et al., Symbiotic crystal-glass alloys via dynamic chemical partitioning, Mater. Today 51 (2021) 6-14.