In this study, the polarization-resolved Raman spectra of b-AsxPx-1 flakes with varying arsenic concentration (x = 0, 0.4, and 0.8) are systematically investigated. A clear polarization dependence is observed in the Raman intensity of all the P-P, As-P, and As-As modes and confirmed by the first-principles calculations. The observed angle-dependence can be related to the structure of the Raman tensors of each peak. In particular, the Raman intensities corresponding to As-P vibration modes are studied in detail. The out of plane As-P mode (Ag1) is clearly identified, but the butterfly-shaped behavior observed in the polar plot around 350 cm−1 is interpreted as the combination of the two in-plane vibrations, one along the armchair and the other along the zigzag direction. This work allows unambiguous assignment of the Ag1, B2g, and Ag2 modes of the As-P vibrational modes and the importance of the consideration of the superposition of the in-plane B2g and Ag2 modes. Such study can be utilized to further characterize the anisotropic structural properties and analyze the local distribution of the As and P in b−AsxP1−x alloys which will play key roles in electronic and optical properties. This methodology can be further extended to alloyed two-dimensional material systems with in-plane anisotropy in general.