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During the last decade, DNA origami nanostructures evolved into versatile platforms for the investigation of numerous biomolecular processes and reactions. [1] This development was initiated by the unique addressability of DNA origami nanostructures, which allows for the site-selective immobilization of multiple biomolecular species with nanometer resolution on the DNA origami surface. Using this approach, a vast variety of biomolecular processes have been investigated so far, including DNA-DNA [2] and DNA-RNA hybridization, [3] protein-DNA binding, [4] conformational transitions in DNA, [5] DNA radiation damage, [6] enzymatic DNA repair, [7] enzyme cascades, [8] antibody-antigen binding, [9-11] and even DNA transcription. [12] The aims of these studies were either to provide fundamental insights into the molecular mechanisms of biological processes or to improve the detection of medically relevant biomolecules. Another class of biomolecular reactions of great importance in a more technological context comprises the binding of proteins to small-molecule ligands, which is at the heart of drug screening and fragment-based drug discovery (FBDD). [13,14] The fundamental idea behind the FBDD approach is to identify and select few low-molecular mass fragments that efficiently bind to neighboring sites of the same target protein and subsequently merge them to construct a potent small-molecule protein inhibitor. [14] The latter step, however, often presents an enormous challenge as the linking chemistry

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