We will show examples of 0D-2D heterostructures connected through covalent and noncovalent chemistry. In the first example, we will show a method to functionalize graphene covalently with exquisite atomic selectivity and yield (NanoLett. 2016, Chem. Commun. 2017). In the second example, we will show that the photoresponse of MoS2 photodetectors can be enhanced by simple and reversible supramolecular functionalization with organic dyes (Chem. Commun. 2016). We will also show the example of a naturally occurring van der Waals heterostructure, franckeite, an air stable, p-doped semiconductor with photoresponse in the far IR (Nat. Comms. 2017). Finally, we will present strategies for the self assembly of liquid-phase exfoliated 2D materials from suspension into functioning electronic devices (Chem. Commun. 2017).