We demonstrate an N2 plasma-enhanced process for inducing (0001)-oriented ALD-grown AlN on planar substrates. We evaluate the impact of {111}-textured Pt as a growth template, precursor chemistry, dose time, stress-engineered substrates, inductively coupled plasma conditions for film bombardment during growth, and ALD equipment configurations. The thin film transverse piezoelectric coefficient e31,f determined from measurements on microelectromechanical system cantilevers coated by PEALD AlN is reported to be −0.53 ± 0.03 C/m2. An analysis of the Pt-AlN interface properties based primarily on depth-profile x-ray photoemission spectroscopy and transmission electron microscopy-energy dispersive spectra is presented. Other than the c axis wurtzite (0001) diffraction peak, no other AlN peaks were observed above the detection limits for XRD measurements. The XRD rocking-curve full-width half-maximum of the 0001 peaks was 2.9° omega, which was achieved on {111}-textured Pt. The relative dielectric constant was measured to be 8.1 < K < 8.6, and an average dielectric loss of < 0.01 was observed within the applied electric field range of ±3350 kV/cm at 10 kHz. The leakage current of the textured AlN was quite low at 1.5 × 10−6 A/cm2 over the applied field range of ±1820 kV/cm.