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Van der Waals layered and 2D materials constitute an extraordinary playground for condensed matter physics, since the strong confinement of wavefunctions to two dimensions supports a diverse set of correlated phenomena. By creating carefully designed heterostructures, these can be readily manipulated. In this Perspective, we advance the viewpoint that heterostructures from these materials with thin layers of organic molecules offer an opportunity for creating and manipulating the correlated degrees of freedom in unprecedented ways. We briefly survey what has been accomplished thus far, including proposed mechanisms, before concentrating on unique opportunities offered by the vast selection of available organic molecules. We further introduce the notion of “proximitization” in combination with symmetry breaking as a fertile and potentially unifying conceptual vantage point from which to consider opportunities for tailoring correlations in van der Waals layered materials.