In recent years, thin metallic films have become object of intense research due to the activation of mechanical size effects enabling a combination of large yield strength and ductility [1]. However, the correlation between microstructure and mechanical behavior is still not fully grasped and the research on new nanostructures with improved mechanical properties is ongoing. In this context, among the physical vapor deposition techniques (PVD), Pulsed Laser Deposition (PLD) have shown a great potential to widely tune the film morphology by simply changing the deposition pressure affecting the growth mechanisms ranging from atom-by-atom to cluster-assembled growth [2]. Nevertheless, very few studies focus on PLD deposited metallic films [3]. Here, I will show the potential of PLD to synthetize two (2) classes of emerging metallic thin films, namely metallic glasses (MGTFs) and high entropy alloys thin films (HEATFs). Firstly, I will cover the results involving the synthesis and the mechanical behavior of ZrCuAlx MGTFs with different compositions (x = 0, 5, 8, 13 %at.) and morphologies i.e. compact and nanogranular. HRTEM shows a unique self-assembled nanolayered structure with local chemical enrichments alternating ZrCu and Al-rich nanolayers. This leads to a large and tunable elastic modulus and hardness, respectively up to 145 and 9.3 GPa. Furthermore, in situ SEM micropillar compression tests show that compact films have outstanding combination of yield strength (3.2 GPa) and ductility (5.5%), among the highest values reported in literature, while nanogranular films show a fully homogenous deformation (up to 20%) with the suppression of the shear bands process. In the second case, I will present new results focusing on AlxCoCrCuFeNi HEATFs deposited by PLD with different compositions (x = 0, 9, 16 %at.) and morphologies, i.e. compact and nanogranular. HRTEM reveal a unique nanolayered structure with nanoscale Al segregations resulting in a nanocomposite FCC/amorphous structure. This leads to enhanced mechanical properties with hardness up to 11 GPa and an exceptionally large (> 3.5%) onset of crack formation when deformed on polymer substrate. Overall, the presented results show the potential of PLD to synthetize a novel class of metallic thin films with large and tunable mechanical properties and potential interest as structural coatings. References : 1. M. Ghidelli et al., Acta Mater., 131, 246, 2017. 2. F. Di Fonzo et al., Nanotechnology, 20, 015604, 2009 3. M. Ghidelli et al., Acta Mater., 213, 116955, 2021