chiral plasmonic nanoparticles and their self-assembled structures as colloidal suspensions. [6][7][8][9] Recently, beyond noble metal plasmonics, solid-state layered nanomaterials that are rotationally aligned with a defined twist angle are becoming increasingly investigated (Figure 1). Among these are twisted 2D van der Waals (vdW) materials, [10][11][12] twisted single-crystal slabs, [13,14] twisted aligned nanowire thin films, [15][16][17][18] and twisted metasurfaces with periodic subunits [19][20][21] (Figure 2). These chiral stacked materials possessing geometric handedness and optical chirality can be seen as truncated and minimalistic versions of supramolecular liquid crystals in the chiral nematic phase or of 3D chiral photonic crystals. [22][23][24] Compared to their bulk or multiple-layer counterparts, the fabrication becomes greatly simplified for bilayer or few-layer chiral metamaterials, enabling precise control over the interlayer twist angle to manipulate lightmatter interactions. Ultrathin chiral metamaterials and metasurfaces with tunable optical and chiroptical responses are thus an active field for study.Twisting achiral layered nanostructures in parallel planes enables engineering of the extrinsic chirality and related optical performance. Specifically, the twist angle from counterclockwise rotation of an upper layer with respect to the beneath one is defined to be positive, θ > 0°, leading to a left-handed stacking geometry. [10,18] Accordingly, negative twist angle from clockwise rotation gives rise to the right-handed counterpart. Accurate control over the interlayer rotation angle offers flexible manipulation of properties, especially optical activity, of twisted layered systems of a wide variety of monolayer constituents and dimensions. A well-studied system is twisted bilayer graphene (TBG), catalyzing the research on twisted stacked nanostructures over the past few years, especially as many intriguing properties of magic-angle graphene are uncovered. [28][29][30] The twist angle dependencies of phonon dispersion, [31] optical absorption and reflection, [32,33] circular dichroism (CD) and birefringence, [10,34] second harmonic generation (SHG), [35] and photoresponse [36,37] of TBG have been extensively explored in the past few years. Similar realizations have been reported for twisted nanostructures of other 2D materials such as transition metal dichalcogenides, [38,39] graphitic carbon nitride, [40] and hexagonal boron nitride (hBN), [41] as well as non-2D systems like polymeric thin films or patterned plasmonic nanohole arrays. [42,43] Therefore, there exists fertile ground for chiral metasurface design Artificial chiral nanostructures have been subjected to extensive research for their unique chiroptical activities. Planarized chiral films of ultrathin thicknesses are in particular demand for easy on-chip integration and improved energy efficiency as polarization-sensitive metadevices. Recently, controlled twisted stacking of two or more layers of nanomaterials, such as 2D van der ...