Optical films and surfaces using geometric phase are increasingly demonstrating unique and sometimes enhanced performance compared to traditional elements employing propagation phase. Here, we report on a diffraction grating with wider angular bandwidth and significantly higher average first-order efficiency than the nearest prior art of metasurfaces, volume holographic gratings, and surface-relief gratings configured to achieve a steep deflection angle. More specifically, we demonstrate a liquid crystal (LC) polymer Bragg polarization grating (PG) with large angular bandwidth and high efficiency in transmission-mode for 532 nm wavelength and 400 nm period. Angular bandwidth was significantly increased by arranging two slanted grating layers within the same monolithic film. First, we studied the optical properties with simulation and identified a structure with 48° angular bandwidth and 70% average first-order efficiency. Second, we fabricated a sample using a photo-aligned chiral nematic LC, where the two grating slants were controlled by the chiral dopants. We measured 40° angular bandwidth, 76% average efficiency, and 96% peak efficiency. Strong input polarization sensitivity (300:1 contrast) and spectral bandwidth (200 nm) mostly matched prior PGs. This approach is especially advantageous for augmented-reality systems and nonmechanical beam steering.