We present results of our first principle and experimental study on new Heusler alloys candidates for half-metallic electrode and nonmagnetic spacer in current-perpendicular-to-plane giant magneto-resistance devices. The electronic structures of Fe2CrSi and Cu2CrAl are characterized by high density of states at the Fermi level in the majority spin band with a good match in their majority band structures near the Fermi level. The calculated interfacial spin polarization in Fe2CrSi/Cu2CrAl (100) superlattice is ∼80%. We have also epitaxially grown ferromagnetic A2 Fe-Cr-Si and nonmagnetic L21 Cu-Cr-Al (100) films on Cr-buffered MgO(100) substrates.