Combinatorial arc plasma deposition (CAPD) method was used to search for new compositions of thin film amorphous alloys. A cathodic arc plasma gun (APG) was adopted as the deposition source for CAPD. The CAPD setup has three APGs radiating out from the center of a substrate. The APGs shoot pulse-like plasma shots one by one at a specific time interval. The plasma from each APG cathode is guided onto a specific area on a substrate by a magnetic field. Each such area overlaps the adjacent ones. Thus, a compositionally-graded thin film is deposited in the overlap area because of mixing of each deposited thin film from each APG that has a thickness grade. The deposited thin film is separated into 1,089 samples (the size of each is 1×1 mm2) using a grid on the substrate. The samples together are referred to as the thin film library. To demonstrate the capability of CAPD, two thin film libraries were deposited in this study. One is a thin film library of a PdCuSi alloy system, and the other is a MoZrPd system. The compositions and crystallinity of the samples were evaluated on the substrate using EDS and IP-XRD respectively. Analysis of the samples showed a graded composition, and some of the samples were shown to be amorphous in both libraries.