Thorium as a potential nuclear fuel for the next-generation thorium-based molten salt reactors holds significant environmental and economic promise over the current uranium-based nuclear reactors. However, because thorium (Th 4+ ) usually coexists with other rare earth elements, alkali or alkaline earth metals in minerals, or highly acidic radioactive waste, seeking acidresistant sorbents with excellent selectivity, high capacity, and fast removal rate for Th 4+ is still a challenging task. In this work, we investigated a robust layered metal sulfide (KInSn 2 S 6 , KMS-5) for Th 4+ removal from strong acidic solutions. We report that KMS-5 could capture Th 4+ from a 0.1 M HNO 3 solution with extremely high efficiency (∼99.9%), fast sorption kinetics (equilibrium time < 10 min), and large distribution coefficient (up to 1.5 × 10 6 mL/g). Furthermore, KMS-5 exhibited excellent sorption selectivity towards Th 4+ in the presence of large amounts of competitive metal ions like Eu 3+ , Na + , and Ca 2+ . This extraordinary capture property for Th 4+ is attributed to the facile ion exchange of Th 4+ with K + in the interlayers and subsequent formation of a stable coordination complex via Th−S bonds. These results indicate that KMS-5 is a promising functional sorbent for the effective capture of Th 4+ from highly acidic solutions.