Biological catch bonds exhibit unique mechanical properties that strengthen with tension. This characteristic in selected receptor-ligand interactions underpins vital biological functions, including adhesion dynamics, cell communication, and mechanosensing. Despite decades of discoveries and modelling, an artificial catch bond has yet to be created. We present the “fish-hook”, the first rationally designed catch bond using DNA. Two mechanically distinct dissociation pathways were designed such that the weak pathway is favoured at low forces and the strong one at high forces. We developed models to design these DNA structures and experimentally validated the catch bond behaviour by single-molecule force spectroscopy. The fish-hook architecture supports a vast sequence and behaviour space, making this a valuable tool for reprogramming biological interactions and engineering novel materials.