Hierarchical Self-Assembled Crystals: Self-assembled crystalline structures achieve a well-defined order without the need to control the position of the individual structure components. Hierarchical crystals possessing two distinct feature sizes, like the ones shown, were fabricated through self-assembly and capillary peeling. A 2 μm sphere monolayer was self-assembled and then transferred to a water-air interface. The floating monolayer was then coated conformally on a 10 μm sphere self-assembled monolayer. Structures like these have the potential to be used in extreme thermal management applications, enabling next-generation electronics that dissipate heat fluxes comparable those present at the surface of the sun. Contributors: Carlos D. Díaz-Marín, Diane Li, Fernando. Vázquez-Cosme, Simo Pajovic, Hyeongyun Cha, Youngsup Song, Cameron Kilpatrick, Geoffrey Vaartstra, Chad Wilson, Svetlana Boriskina, Evelyn N. Wang