the chiral light-matter interactions include two distinct phenomena: circular dichroism characterized by the absorption difference between transmitted left circularly polarized (LCP) and right circularly polarized (RCP) lights [4] and circular birefringence caused by phase accumulation difference between LCP and RCP lights. [5] Recently, chirality induced by artificial nanostructures and their 3D arraysmetamaterials has drawn much attention in the scientific community due to the arbitrary symmetric design and abundant optical resonance engineering of nanostructures. Such effects enable significant polarizability tensor manipulation of the optical fields with high degree of freedom (DOF). [6] Based on different local chiral electromagnetic resonances of the nanostructures, researchers have developed numerous functional chiral designs such as chiral biosensing, [7] chiral bound states in the continuum, [8] Janus plasmonic helical nanoapertures, [9] and weak chirality for strong coupling between resonant states. [10] In the past decade, metasurfaces as planar counterparts of metamaterials have been extensively investigated due to their exotic electromagnetic properties for efficient scattering control of the electromagnetic waves. [11][12][13][14][15] In contrast to conventional optics, metasurfaces consist of arrays of subwavelength elements ("meta-atoms") that can locally manipulate light−matter interactions. Spatially varying meta-atoms allow the control of the polarization, phase, and amplitude of light, leading to high DOF to manipulate the electromagnetic waves from near-fields to far-fields. [16,17] The light−matter interactions supported by the meta-atoms include local multi-polar resonances [18,19] and near-field coupling resonances such as Fano resonances [20] and bound states in the continuum. [21,22] Generally, such resonances are accompanied by enhancement of local electric or magnetic fields, leading to enhanced nonlinear responses such as second harmonic generation (SHG) and third harmonic generation (THG). [23][24][25] Although the overall nonlinear efficiency of the reported metasurfaces is still not comparable to that in conventional nonlinear crystals, the nonlinear efficiency of metasurfaces is much higher when considering their planar nature. Most importantly, metasurfaces provide an efficient platform for optical frequency mixing and high harmonic generation. [26][27][28] On the other hand, based on a variety of local resonances of meta-atoms, metasurfaces can be designed to carry different Optical chirality, which describes the property of asymmetric light-matter interactions for different handedness of polarization, plays an important role in physical photonics, biochemical processes, and molecular recognition. Recently, asymmetric optical responses of chiral nanostructures provide a wide platform for arbitrary and artificial manipulation of optical chirality. Here, a design strategy is theoretically and experimentally introduced to realize a spin-selective coding metasurface in both linear a...