Small-scale mechanical testing techniques can now obtain reliable, high-quality mechanical properties data from very small volumes of material. Here, we use such techniques to probe the uniaxial tension and compression response of nanostructured metals with embedded intergranular films. These hierarchical materials are predicted to have a unique combination of strength and ductility, but require onerous processing routes for fabrication of bulk samples. Microtensile and microcompression experiments are used to obtain quantitative stress-strain curves from these nanostructured alloys, allowing us to quickly revisit the materials processing tasks and speed materials discovery. We report on the yield, strain hardening, and fracture of these materials, with a specific focus on understanding strain localization and catastrophic failure.