Swift electrons moving closely parallel to a periodic grating produce far-field radiation of light, which is known as the Smith-Purcell effect. In this letter, we demonstrate that designer Babinet metasurfaces composed of C-aperture resonators offer a powerful control over the polarization state of the Smith-Purcell emission, which can hardly be achieved via traditional gratings. By coupling the intrinsically nonradiative energy bound at the source current sheet to the out-of-plane electric dipole and in-plane magnetic dipole of the C-aperture resonator, we are able to excite cross-polarized light thanks to the bianisotropic nature of the metasurface. The polarization direction of the emitted light is aligned with the orientation of the C-aperture resonator. Furthermore, the efficiency of the Smith-Purcell emission from Babinet metasurfaces is significantly increased by 84%, in comparison with the case of conventional gratings. These findings not only open up a new way to manipulate the electron-beam-induced emission in the near-field region but also promise compact, tunable, and efficient light sources and particle detectors. DOI: 10.1103/PhysRevLett.117.157401 Metasurfaces, two-dimensional metamaterials, have recently emerged as a new frontier of science because they provide large degrees of freedom to control over the propagation of light [1]. Metasurfaces allow us to tailor the phase, amplitude, polarization, and ray trajectory [2-4] of light based on a single layer of engineered structures or meta-atoms [5][6][7]. Conventional optical devices usually rely on phase accumulation over a long optical path due to the inherently weak interaction of light and matter. Metasurfaces, in contrast, provide an elegant way to overcome the constraint by designing suitable subwavelength meta-atoms and arranging their spatial distributions in a prescribed manner to regulate the local light-matter interactions. This new methodology has enabled numerous novel optical phenomena and devices on a planar platform, including unidirectional coupling of surface plasmon polaritons [8][9][10], information processing [11], spin-orbit manipulation [12,13], highly efficient holography [14], and an ultrathin invisibility cloak [15]. Metasurfaces have also been employed in nonlinear optics, where they provide promising approaches to control the nonlinearity phase [16] and amplify the efficiencies of nonlinear processes [17,18].The interaction of swift electrons with a material can generate far-field electromagnetic radiation that is coherent to the evanescent field associated with the moving electrons. This effect is well known as electron-induced emission [19]. The analysis of various interactions between electrons and materials is a substantial source of inspiration for advanced electron microscopy, including electron energy-loss spectroscopy, and cathodoluminescence emission, including transition radiation, Cherenkov radiation, and diffraction radiation. Recent breakthroughs in artificially engineered metamaterials and nanotechnology...