Combinatorial methodology offers an efficient platform to accelerate the exploration of new materials. We demonstrate the effectiveness of this technique on the study of new metal gates for the advanced gate stack. We report two examples, Ni-Ti-Pt ternary composition spreads, and Tai.xAl xNy binary composition spreads, using a combinatorial sputtering tool. For the Ni-Ti-Pt library, wavelength dispersive spectroscopy (WDS), and scanning x-ray microdiffraction spectroscopy were used to determine compositions, and structures, respectively. Scanning Kelvin probe microscopy (SKPM) was used to measure work functions (Φm) directly. Our results show Φm variation is consistent with the variation for the corresponding bulk values. For the Tai.xAlxN y metal gate electrodes, the extracted equivalent oxide thickness (EOT) map suggests thermal stability of the stack, and flat-band voltage shift (△Vfb) varied systematically as per our expectation.