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New technologies are emerging which allow us to manipulate and assemble 2-dimensional (2D) building blocks, such as graphene, into synthetic van der Waals (vdW) solids. Assembly of such vdW solids has enabled novel electronic devices and could lead to control over anisotropic thermal properties through tuning of inter-layer coupling and phonon scattering. Here we report the systematic control of heat flow in graphene-based vdW solids assembled in a layer-by-layer (LBL) fashion. In-plane thermal measurements (between 100 K and 400 K) reveal substrate and grain boundary scattering limit thermal transport in vdW solids composed of one to four transferred layers of graphene grown by chemical vapor deposition (CVD). Such films have room temperature in-plane thermal conductivity of ~400 Wm⁻¹ K⁻¹. Cross-plane thermal conductance approaches 15 MWm⁻² K⁻¹for graphene-based vdW solids composed of seven layers of graphene films grown by CVD, likely limited by rotational mismatch between layers and trapped particulates remnant from graphene transfer processes. Our results provide fundamental insight into the in-plane and cross-plane heat carrying properties of substrate-supported synthetic vdW solids, with important implications for emerging devices made from artificially stacked 2D materials.

Advancements in 3D additive manufacturing have spurred the development of effective patient‐specific medical devices. Prior applications are limited to hard materials, however, with few implementations of soft devices that better match the properties of natural tissue. This paper introduces a rapid, low cost, and scalable process for fabricating soft, personalized medical implants via stereolithography of elastomeric polyurethane resin. The effectiveness of this approach is demonstrated by designing and manufacturing patient‐specific endocardial implants. These devices occlude the left atrial appendage, a complex structure within the heart prone to blood clot formation in patients with atrial fibrillation. Existing occluders permit residual blood flow and can damage neighboring tissues. Here, the robust mechanical properties of the hollow, printed geometries are characterized and stable device anchoring through in vitro benchtop testing is confirmed. The soft, patient‐specific devices outperform non‐patient‐specific devices in embolism and occlusion experiments, as well as in computational fluid dynamics simulations.