We report an improved method for depositing Heusler alloy thin films, which reduces the B2-ordering temperature, and demonstrate its effect on improving spin-polarization and ΔR/R in CPP-GMR sensors. The insertion of a CoFeBTa or CoBTi amorphous ferromagnetic underlayer induced the formation of an amorphous Co2(Mn,Fe)Ge Heusler alloy film, reducing the B2-ordering temperature to ∼220 °C, which is significantly lower than the value of 500 °C for an epitaxial system and 400 °C for a polycrystalline system. This novel approach allows the fabrication of spin-valve sensor structures with ΔR/R of 18% after post-deposition annealing at temperatures less than 300 °C and is thus compatible with standard recording read-head sensor production.