Nowadays, flexible electronics are rapidly developing with the continuous search for novel materials with large electrical and mechanical properties [1]. Thin film metallic glasses (TFMGs) are appealing candidates due to their high mechanical properties, low and negative temperature coefficient of electrical resistivity, stability of electrical resistivity with thickness variation, and good fatigue resistance. However, their employment in flexible electronics is still limited due to their high electrical resistivity vs crystalline materials, and their macroscopically brittle behavior mediated by shear bands (SBs) [2]. Nanostructuring strategies can hinder these downsides. For example, nanolaminates with 120 nm-thick layers of amorphous Zr50Cu50 and 16 nm-thick nanocrystalline Cu reached a tensile strength of ~2.5 GPa and fracture strain up to ~4% [3]. Nevertheless, unresolved scientific issues are still present involving the understanding of the deformation mechanisms for nanostructured crystal/glass and the development of effective synthesis strategies to improve the mechanical and electrical properties simultaneously. Here, we synthesize crystal/glass nanolaminates and nanocolumnar TFMGs with large and controlled mechanical and electrical properties. Firstly, we will focus on the fabrication of Fe/ZrCu crystal-(BCC)/glass nanolaminates, with different ZrCu fractions from 0.5 up to 0.9 and bilayer periods from 10 up to 40 nm. Among the main results, we will show that micropillar compression tests on 40/40 nm Fe/ZrCu multilayers showed a yield strength of ~5 GPa and a strain of up to 9% without failure due to the presence of crystal/glass interfaces hindering the SBs propagation. Moreover, tensile tests on samples deposited on a flexible polymeric substrate presented a crack onset strain (COS) of up to 1.36 %, while reaching an electrical resistivity of 36 µOhm*cm, close to pure Fe, resulting from the presence of continuous Fe-layers effectively enabling the electrons transport. Secondly, we will focus on the synthesis of ZrCu nanocolumnar TFMGs with nanocolumn diameters from 16 up to 60 nm [4]. Among the main results, we show a trade-off between nanocolumn size and COS, with the largest values obtained for a 60 nm-diameter column, reporting low electrical resistivity of 280 µOhm*cm and the highest COS value of 1.6 %, even larger than their monolithic counterparts (1.35%). This results from the reduced electron scattering with nanocolumn interfaces, which also accommodate larger plastic deformation, delaying the formation of shear bands. Overall, our findings highlight the impact of synthesis strategies on controlling the mechanical and electrical properties of nanostructured TFMGs, increasing their potential in flexible electronics. 1. Corzo, D., Tostado-Blázquez, G. & Baran, D. Frontiers in Electronics 1, (2020). 2. Lee, S. et al., Skin Heat Patches. Nano Lett 20, 4872–4881 (2020). 3. Kim, J. Y., Jang, D. & Greer, J. R. Adv Funct Mater 21, 4550–4554 (2011). 4. Boltynjuk, E. et al. submitted to Script Mater (2024).