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Supramolecular engineering comprises the design, synthesis and self-assembly of well-defined molecular modules into tailormade architectures. The incorporation of functional units in these molecular modules makes it possible to provide a preprogrammed function to the overall architecture and material, thus paving the way towards its technological application in a myriad of fields.[1] For this purpose, the last decade has witnessed an increasing interest towards the 3D engineering of supramolecular materials.[2–6] The colossal task of achieving full control over self-assembled systems however, is the ongoing endeavor of the supramolecular scientists and to date only few systems may be pre-programmed to undergo controlled self-assembly in 3D.[7–11] In contrast, 2D interfaces provide a simplified platform for supramolecular and crystal engineering, and the field has known an exciting growth.[12–15] These …