Materials possessing sub-micrometer scale features often show unique mechanical properties combining large yield strength and ductility due to the activation of size effects [1]. However, the correlation between microstructure and mechanical properties is not fully grasped and the research of new nanostructures with unconventional properties or enhanced performances is subject of intense research. In this context, pulsed laser deposition (PLD) has great potential to tune the film nanoscale morphology and atomic structure (e.g. degree of disorder/crystallinity) by simply adjusting synthesis parameters, e.g. the deposition pressure, leading to atom-by-atom or cluster-assembled growth regimes, resulting in compact and nanogranular films, respectively [2]. Nevertheless, the use of PLD for the depositing nanostructured metallic films is still in a preliminary phase [3]. Here, I will show my results regarding two classes of films: thin film metallic glasses (TFMGs) and complex compositionally alloys (TF-CCAs). Firstly, I will cover the results involving the synthesis and the mechanical behavior of (ZrCu)100-xAlx TFMGs with different compositions (x = 0, 5, 8, 13 %at.) and morphologies i.e. compact and nanogranular. HRTEM shows a self-assembled nanolayered structure with local chemical enrichments alternating ZrCu and Al-rich nanolayers. This leads to large and tunable elastic modulus E and hardness H, up to 145 and 9.3 GPa, respectively. Furthermore, in situ SEM micropillar compression tests show that compact films have an outstanding combination of yield strength (3.2 GPa) and ductility (5%), among the highest values reported in literature, while nanogranular films show homogenous deformation after yielding (up to 6%) due to their structural heterogeneity which delays the maturation of shear bands like in nanoglasses [4]. Then, I will present results concerning Alx(CoCrCuFeNi)100-x TF-CCAs with different compositions (x = 0, 9, 16 %at.) and morphologies. CoCrCuFeNi films possess an FCC nanocrystalline structure leading to enhanced H (up to 12 GPa) with respect to sputter-deposited films. In addition, CoCrCuFeNi reports an exceptionally high (>3.5%) onset of crack formation when deformed on polymer substrates because of the high energy of the deposition process, leading to strong adhesion and preventing crack activation and percolation. Furthermore, HRTEM of Alx(CoCrCuFeNi)100-x reveals a nanolaminated structure alternating segregated Al (2 nm) and CoCrCuFeNi alloy (5 nm), which induces a slight decrease of E (from 175 to 160 GPa) and H (from 12 to 9.5 GPa) vs the base CCA due to a combination of the low mechanical properties of Al and, possibly, an inverse Hall-Petch effect caused by the low dimensions of the crystallites inside the nanolayers. Overall, the presented results show the potential of PLD to synthetize a novel class of nanostructured thin metallic films with large and tunable mechanical properties and potential interest as structural coatings. References: [1] M. Ghidelli et al., Acta Mater., 2017; [2] F. Di Fonzo et al., Nanotechnology, 2008; [3] M. Ghidelli et al., Acta Mater., 2021; [4] S. H. Nandam et al., J. Mater. Res., 2021.