Robust and escalating computing demand over the next several decades will necessitate the development of new materials, algorithms, and devices that address both performance and sustainability. We perform advanced materials synthesis, spectroscopy, and device integration focused on new classes of two-dimensional (2D) materials. These planar, few-atom thick 2D crystals and their assemblies exhibit intriguing phenomena that can be harnessed for optics, sensing, energy conversion, quantum control, and of course information technology. In this talk, I will summarize our research advances in 2D atomic crystals, 2D molecular lattices, and the first assembly of bespoke van der Waals heterostructures with these materials. First, I will share how careful control of precursor flux and substrate interactions can both shape and significantly reduce defects in 2D transition-metal dichalcogenide (TMD) crystals that show promise as building-blocks for future field effect transistors. Second, I will show how our unique capabilities in gas-phase synthesis and exfoliation of 2D metal-organic frameworks (MOFs), which harbor stimulus responsive properties and mixed-valency, enable the creation of unconventional sensors and catalytically-active substrates. Finally, I will discuss how seamless integration of 2D TMD monolayers with molecular thin films and 2D MOFs yields devices that exhibit efficient photon upconversion and unprecedented quantum emission phenomena. Collectively, these efforts help address some of the essential materials needs critical to future computer hardware.