Electrically conductive metal–organic frameworks (MOFs) are important due to their applications in electrocatalysis, energy storage, and electronic devices. However, their synthesis is often poorly developed, resulting in small crystal sizes and a limited understanding of their physical properties. I hypothesize that a critical barrier to their synthesis is uncontrolled ligand oxidation, as conductive MOFs often contain air-sensitive catechol, o-phenylenediamine, and dithiolene building units. During this award period, I will examine the synthesis of π–d conjugated 2D frameworks, an important family of conductive MOFs, via controlled chemical oxidation in an inert atmosphere. I will optimize my synthetic parameters using a design of experiments approach, in order to identify trends between a multitude of variables. Future work will focus on in situ studies to model crystal nucleation and growth. Ultimately, my goal is to gain control over size and shape of 2D MOFs to better understand their properties and enable device integration.