A high-throughput multi-plume pulsed-laser deposition (MPPLD) system has been demonstrated and compared to previous techniques. Whereas most combinatorial pulsed-laser deposition (PLD) systems have focused on achieving thickness uniformity using sequential multilayer deposition and masking followed by post-deposition annealing, MPPLD directly deposits a compositionally varied library of compounds using the directionality of PLD plumes and the resulting spatial variations of deposition rate. This system is more suitable for high-throughput compound thin-film fabrication.