We report here the first pharmaceutical twistable hydrogen-bonded two-dimensional plastic hydrate crystal of a well-known psychoactive drug, caffeine (CAH). The availability of two pairs of plastically bendable faces in orthogonal directions allows for twisting of the CAH crystals to obtain the helical morphology. We further demonstrate the first pharmaceutical application of such twistable crystals, i.e., exceptional tabletability. The plasticity of CAH is comparable to a commonly used highly plastic tablet diluent, microcrystalline cellulose. This example suggests that the strategies for designing twistable crystals, among other potential applications, can be used to effectively overcome compression problems of certain drugs and enable the development of high-quality drug tablets.
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