The microstructure and mechanical properties of Cu46.5Zr48.5Al5 and Cu50Zr50 rods are investigated. Cu50Zr50 is composed of nanostructured martensitic phases, while the Cu46.5Zr48.5Al5 alloy comprises micrometer-sized dendrites (mainly austenitic phase) in an amorphous matrix. Both samples show considerable plasticity under compression and a work-hardening ability. Martensitic phase transformations during deformation play a significant role with regard to the mechanical properties. Nanoindentation tests on the different phases comprising the alloys indicate that the amorphous matrix in Cu46.5Zr48.5Al5 is harder than the crystalline phases and has a less-pronounced indentation-size effect.