A significant experimental challenge in testing proposed relationships between structure and properties is the synthesis of targeted structures with atomistic control over both the structure and the composition. SnSe2(MoSe2)1.32 was synthesized to test the hypothesis that the low-temperature synthesis of two interleaved structures would result in complete turbostratic disorder and that the disorder would result in ultralow thermal conductivity. SnSe2(MoSe2)1.32 was prepared by depositing elements to form a precursor containing Sn|Se and Mo|Se bilayers, each containing the number of atoms required to form single dichalcogenide planes. The nanoarchitecture of alternating Sn and Mo layers is preserved as the dichalcogenide planes self-assemble at low temperatures. The resulting compound contains well-formed dichalcogenide planes that closely resemble that found in the binary compounds and extensive turbostratic disorder. As expected from proposed structure–property relationships, the thermal conductivity of SnSe2(MoSe2)1.32 is ultralow, ∼0.05 W m–1 K–1.