in plasmonic metasurfaces. [24] Compared to the conventional quadratic nonlinear optical materials such as ferroelectric crystals, nonlinear plasmonic metasurfaces can continuously control the local phase shift of effective nonlinear polarizability in the entire 2π range with subwavelength resolution for nonlinear wavefront shaping. [14] Among various applications of metasurfaces, the generation of optical vortex beam with helical wavefront carrying orbital angular momentum (OAM) has attracted great interests. [8,11,[25][26][27][28][29] Compared to the conventional bulky optical components used for generating vortex beams, such as spatial light modulator and spiral phase plate, metasurfaces provide a compact and high-resolution approach, which open new avenues for optical particle trapping, [30,31] precision photolithography, [32,33] and remote optical communication. [34,35] Furthermore, the generation of secondharmonic (SH) vortex beams have been recently achieved with both the fork-type and rotation plasmonic metasurfaces, [19,21] but the formed SH vortex beams can only carry OAM of one absolute value and the vortex mode purity is still limited. Besides, the fork-type metasurface demonstrates no spin control over the created SH vortex pair, [19] while the rotation metasurface can only generate one vortex beam with the opposite spin at one time. [21] Moreover, most of the existing nonlinear plasmonic metasurfaces employ metallic nanoantennas as their constitutional meta-atoms, which suffer from strong background transmission, undesired optical scattering, and low laser damage threshold. As a solution, Babinet-inverted plasmonic metasurfaces based on nanoapertures in metallic film as nonlinear meta-atoms have their unique advantages, where the transmission of background illumination and undesired optical scattering can be efficiently suppressed, resulting in a significantly improved signal-to-noise ratio for the nonlinear beam conversion. [36] Meanwhile, the generated Joule heat in Babinetinverted plasmonic metasurfaces under the femtosecond laser illumination can diffuse rapidly across the continuous metallic film with high thermal conductivity, leading to a high laser damage threshold. [37,38] In this work, we present Babinet-inverted plasmonic metasurfaces based on C-shaped nanoapertures for achieving strong SH emission with large nonlinear conversion efficiency and generating spin-selective SH vortex beams with high mode purity. The geometrical parameters of C-shaped nanoapertures, Metasurfaces have drawn considerable attentions for their revolutionary capability of tailoring the amplitude, phase, and polarization of light. By integrating the nonlinear optical processes into metasurfaces, new wavelengths are introduced as an extra degree of freedom for further advancing the device performance. However, most of the existing nonlinear plasmonic metasurfaces are based on metallic nanoantennas as meta-atoms, suffering from strong background transmission, low laser damage threshold and small nonlinear conversion e...