Huang, Ting-ChunTing-ChunHuangChen, Yu-XinYu-XinChenChen, Yu-LinYu-LinChenWu, Meng-TingMeng-TingWuPai, Chi-FengChi-FengPaiChuang, ChiashainChiashainChuangHsieh, Ya-PingYa-PingHsiehHofmann, MarioMarioHofmann2026-01-262026-01-262025-11-19https://scholars.lib.ntu.edu.tw/handle/123456789/735592Two-dimensional (2D) transition-metal dichalcogenides (TMDCs) offer band alignments that are well-suited for minority-spin filtering when interfaced with ferromagnets. Unfortunately, interfacial hybridization results in the emergence of metallic states in MoS2that have limited previous results significantly below theoretical expectations. Here, we study the metallization at the Co/MoS2interface and devise a method to overcome its detrimental impact on spin transport. Using a contamination-free fabrication process, clear evidence of hybridization was observed, which increases the magnetic anisotropy of the interface. Magneto-transport and theoretical analysis reveal that the metallic wave functions extend into the MoS2layer, suppressing its ability as a filter barrier. The spin-filtering ability can be restored when separating the MoS2by only two atomic layers. The resulting device achieves a record tunneling magnetoresistance (TMR) of −170.2%, consistent with simulations of ideal minority spin filtering. Temperature-dependent measurements further distinguish two dominant transport regimes, spin injection at low temperatures and spin-dependent tunneling at higher temperatures. The combined contribution of these mechanisms sustains high TMR across the full temperature range. Our findings establish a path for realizing scalable, high-performance 2D spintronic devices for applications in MRAM, spin logic, and magnetic sensing.magnetic tunnel junctionmagnetoresistancemetalizationMoS2spin filterjournal article10.1021/acsami.5c15955