The advances in nanotechnology have pushed materials science to the point where structural control at atomic precision is becoming feasible. This appears to mark the ultimate reachable limit for the atomistic design of materials with predestined properties, which are ⴕ These authors contributed equally to this work 2 defined by chemical composition and bonding. Fundamentally different to this classical design approach is the manipulation of the material's properties without changing the chemical bonding network, for example by applying strain or by twisting the layers of stacked two-dimensional (2D) crystals with respect to one another. Indeed, twisting van der Waals homo-and heterolayers of 2D crystals against each other has proven to alter the electronic properties of these materials and is commonly referred to as twistronics. The relation between the twist angle, 𝜃, which also determines the moiré cell size (see Fig. ), and the electronic properties has been predicted and demonstrated for bilayers (BLs) of graphene and transition-metal dichalcogenides ].