Abstract : In article number 1900551, Ran Ang and co‐workers report strong anisotropic thermal conductivity in polycrystalline layers of Ag x Sn1‐ x S)1.2 (TiS2 )2 alloys. The researchers report that these properties originate from the natural intercalated structure of the materials. Additionally, Ag substitution at the Sn sites within the SnS phonon barrier layer induces an enhancement of thermoelectric performance, suggesting a new method for thermoelectric manipulation via anisotropy engineering.