Controlling the polarization states of light is of fundamental importance in modern photonic applications. In article number 1901448, Shengyan Yang, Changzhi Gu and co-workers have developed a novel folded metamaterial that possesses gigantic intrinsic 3D chirality and simultaneously supports multispectral spin-dependent transmission. A remarkable circular dichroism approaching unity is experimentally achieved, with >93% of the selected circularly polarized light being transmitted. The folded metamaterials provide an appealing platform for versatile photonic applications in multiband circular polarizers, polarization transformers, chiral imaging, and optical information processing.