Novel high-performance nanostructured films with superior mechanical/electrical properties are required for advanced applications such as micro-/nanoelectronics, energy production, sensors and wear protection. Especially, mutually excluding structural properties such as high strength and ductility need to be combined, but also low electrical resistance enabling reduction of energy losses. In order to trigger microstructure-induced material properties, control of the micro-scale porosity, atomic composition, average grain size, and layer/film thickness must be optimized based on nanoengineering design concepts. In addition, measuring the properties of thin films (thickness ~1 m) requires the development of novel techniques capable to probe their mechanical/electrical behavior. Here, I will present recent results for several class of advanced materials including nanostructured metallic glasses, high entropy alloys and multilayers, highlighting their micro-scale mechanical behavior[1, 2], while I will discuss the measurement of electrical properties across grain boundaries for Cu films[3, 4]. Special emphasis will also be dedicated to present several cutting-edge techniques used to extract the mechanical/electrical behavior at the micro- and nanometer scale, involving in-situ SEM micro-pillar compression, tensile test in-situ TEM, and in-situ SEM electrical resistivity measurements. Finally, I will present recent developments within LSPM, highlighting new research activities dealing with the synthesis of nanostructured metallic films and the development of a new platform for in situ SEM mechanical-electrical characterization. [1] M. Ghidelli et al., Acta Mater. 213 (2021) 116955. [2] G. Wu, C. Liu, A. Brognara, M. Ghidelli, Y. Bao, W. Lu, G. Dehm, D. Raabe, Z. Li, Mater. Today 51 (2021) 6-14. [3] H. Bishara, S. Lee, T. Brink, M. Ghidelli, G. Dehm, ACS Nano 15(10) (2021) 16607-16615. [4] H. Bishara, M. Ghidelli, G. Dehm, ACS Appl. Electron. Mater. 2(7) (2020) 2049-2056.