While ultrasmooth 2D c-MOF films have demonstrated enhanced charge mobility within the conjugated plane, it is equally imperative to enhance the interlayer pathways for out-of-plane charge transport in three dimensions. This can be achieved through the strategic expansion of conjugated systems, optimization of stacking models, and modification of functional groups. Moreover, there is an urgent need to develop alternative and simpler synthesis methods for defect-free single-crystal thin films, addressing the challenges of low yield and harsh synthesis conditions associated with chemical vapor deposition (CVD) and subsequent separation and washing processes involving gallium. Finally, the integration of density functional theory calculations with machine learning approaches could be a great opportunity in predicting and synthesizing the next generation of conductive 2D c-MOFs.