Fischer-Tropsch synthesis (FTS), a significant reaction for effective H2 utilization, is a promising approach for direct production of light olefins from syngas (H2 + CO). For the FT-Olefin process, an efficient catalyst restricting the product distribution of FTS to light olefins is required. Aligned with this goal, we synthesized 24 catalysts comprising Fe and Cu in combination with rare earth metals (La, Ce, Nd, Ho, Er) and zeolite supports (ultrastable Y and mordenite). FT-Olefin performances of these catalysts were screened using a high-throughput test system at atmospheric pressure, and then promising catalysts were tested under high pressure in a conventional test system. Results show that Nd increases selectivity to light olefins and Ho suppresses C5+ and coke formation. It is also demonstrated that zeolite-metal interaction, leading to a mixture of both acidic and basic sites, is significant in increasing light olefin production. The mordenite-supported 20 wt % Fe, 0.5 wt % Cu, and 0.5 wt % Ho catalyst provides the highest light olefin yield with the lowest coke and heavier hydrocarbon selectivity.