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Metals containing abundant coherent twin boundaries (TBs) are able to sustain substantial plastic deformation without fracture due to shear-induced TB migration and sliding. Retaining ductility in these metals, however, has proven difficult because detwinning rapidly exhausts TB migration mechanisms at large deformation, whereas TB sliding was only evidenced for loading on very specific crystallographic orientations. Here, we reveal the intrinsic shear deformability of twins in nanocrystals using in situ nanomechanical testing and multiscale simulations and report extreme shear deformability through TB sliding up to 364%. Sliding-induced plasticity is manifested for orientations that are generally predicted to favor detwinning and shown to depend critically on geometric inhomogeneities. Normal and shear coupling are further examined to delineate a TB orientation-dependent transition from TB sliding to TB …