We conducted a high-throughput investigation of the fundamental properties of (Mg,Hf)_xAl_1–xN thin films (0 < x < 0.24) aiming for developing high-performance AlN-based piezoelectric materials. For the high-throughput investigation, we prepared composition-gradient (Mg,Hf)_xAl_1–xN films grown on a Si(100) substrate at 600 °C by cosputtering AlN and MgHf targets. To measure the properties of the various compositions at different positions within a single sample, we used characterization techniques with spatial resolution. X-ray diffraction (XRD) with a beam spot diameter of 1.0 mm verified that Mg and Hf had substituted into the Al sites and caused an elongation of the c-axis of AlN from 5.00 Å for x = 0 to 5.11 Å for x = 0.24. In addition, the uniaxial crystal orientation and high crystallinity required for piezoelectric materials to be used as application devices were confirmed. The piezoelectric response microscope indicated that this c-axis elongation increased the piezoelectric coefficient almost linearly from 1.48 pm/V for x = 0 to 5.19 pm/V for x = 0.24. The dielectric constants of (Mg,Hf)_xAl_1–xN were investigated using parallel plate capacitor structures with ∼0.07 mm² electrodes and showed a slight increase by substitution. These results verified that (Mg,Hf)_xAl_1–xN is a promising material for piezoelectric-based application devices, especially for vibrational energy harvesters.