Biomagnetic field sensors based on AlN/FeCoSiB magnetoelectric (ME) composites desire a resonant frequency that can be precisely tuned to match the biomagnetic signal of interest. A tunable mechanical resonant frequency is achieved when ME composites are integrated onto shape memory alloy (SMA) thin films. Here, high-quality c-axis growth of AlN is obtained on (111) Pt seed layers on both amorphous and crystallized TiNiCu SMA thin films on Si substrates. These composites show large piezoelectric coefficients as high as d33,f= 6.4 pm/V ± 0.2 pm/V. Annealing the AlN/Pt/Ta/amorphous TiNiCu/Si composites to 700 °C to crystallize TiNiCu promoted interdiffusion of Ti into the Ta/Pt layers, leading to an enhanced conductivity in AlN. Depositing AlN onto already crystalline TiNiCu films with low surface roughness resulted in the best piezoelectric films and hence is found to be a more desirable processing route for ME composite applications.