High-performance volume holographic gratings are important coupling elements for holographic waveguides, and small angular bandwidth and low average diffraction efficiency are major factors restricting the performance of volume holographic gratings. In this paper, a volume holographic grating with large angular bandwidth and high diffraction efficiency is designed and prepared based on asymmetrical tilt recording. First, we discuss the relationship between the recording parameters and the diffraction efficiency of the volume holographic grating under transverse electric mode light and transverse magnetic mode light to find the range of recording parameters at high average diffraction efficiency. Then, the relationship between the recording parameters in this range and the angular bandwidth of the volume holographic grating is further analyzed, thereby determining the best recording parameters to obtain a volume holographic grating with large angular bandwidth and high diffraction efficiency. The experimental results show that when the incident angle of the reference light is 25° and the incident angle of the signal light is 30°, the angular bandwidth of the prepared volume holographic grating reaches ±14° and the diffraction efficiency is 82%.