Multicomponent alloys pose great challenges for efficiently screening desired composition. Here, we combined high-throughput magnetron-sputtering experiments and CALculation of PHAse Diagrams (CALPHAD) methods to screen NiCrAlYSiTa coatings. The compositionally graded coatings showed increased amorphization with higher Si content, indicated by the steepen T0 curves and enlarged amorphous formation region. For the crystallized coatings, the phase structure transformed from Al- and Cr-rich bcc region to Ni-rich fcc, consistent with our calculated phase diagrams. Owing to the high cohesion energy and strong atomic bonding induced by large atomic radius difference and negative mixing enthalpy, the amorphous coatings exhibited superior hardness (25.8 GPa) and elastic modulus (415.8 GPa) compared to the reported multicomponent coatings. By combining high-throughput experimental and theoretical methods, this work pioneers an integrated framework for rapid development of new multicomponent alloy coatings.