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Artificially engineered 2D materials offer unique physical properties forthermal management, surpassing naturally occurring materials. Here, using vander Waals epitaxy, we demonstrate the ability to engineer extremely insulatingultra-thin thermal metamaterials based on crystalline lattice-mismatchedBi2Se3/MoSe2 superlattices and graphene/PdSe2 heterostructures with exceptionalthermal resistances (70-202 m^2K/GW) and ultralow cross-plane thermalconductivities (0.01-0.07 Wm^-1K^-1) at room temperature, comparable to thoseof amorphous materials. Experimental data obtained using frequency-domainthermoreflectance and low-frequency Raman spectroscopy, supported bytight-binding phonon calculations, reveal the impact of lattice mismatch,phonon-interface scattering, size effects, temperature and interface thermalresistance on cross-plane heat dissipation, uncovering different thermaltransport regimes and the dominant role of long-wavelength phonons. Ourfindings provide essential insights into emerging synthesis and thermalcharacterization methods and valuable guidance for the development oflarge-area heteroepitaxial van der Waals films of dissimilar materials withtailored thermal transport characteristics.

Engineering heat transport across epitaxial lattice-mismatched van der Waals heterointerfaces