Metal-sulfur cubane clusters fill an untapped niche for tunable, electrochemically active building blocks. These clusters exhibit reversible electrochemical properties and are structurally diverse. Fe4S4 clusters represent analogues for important biologically prevalent ferrodoxins, which perform important catalytic processes, such as nitrogen fixation in the nitrogenase enzyme. One notable goal is stabilizing these clusters due to their propensity for oxidation. We aim to utilize the characteristic stability of metal organic and covalent organic frameworks for this goal. Recent reports have shown that Janus-bis N-heterocyclic Carbenes (NHCs) can serve as linkers to assemble Co4S4 clusters. This thesis will delve into previous attempts at utilizing NHCs in the synthesis of metal sulfur cubane cluster frameworks, as well as future efforts towards this goal. Specifically, we show progress towards using covalent organic frameworks (COFs) scaffolds to anchor M4S4 clusters.