Monocrystalline silicon (c-Si) is still an important material related to microelectronics/optoelectronics. The nondestructive measurement of the c-Si material and its microstructure is commonly required in scientific research and industrial applications, for which Raman spectroscopy is an indispensable method. However, Raman measurements based on the specific fixed Raman geometry/polarization configuration are limited for the quantified analysis of c-Si performance, which makes it difficult to meet the high-end requirements of advanced silicon-based microelectronics and optoelectronics. Angle-resolved Raman measurements have become a new trend of experimental analysis in the field of materials, physics, mechanics, and optics. In this paper, the characteristics of the angle-resolved polarized Raman scattering of c-Si under the in-axis and off-axis configurations are systematically analyzed. A general theoretical model of the angle-resolved Raman intensity is established, which includes several alterable angle parameters, including the inclination angle, rotation angle of the sample, and polarization directions of the incident laser and scattered light. The diversification of the Raman intensity is given at different angles for various geometries and polarization configurations. The theoretical model is verified and calibrated by typical experiments. In addition, this work provides a reliable basis for the analysis of complex polarized Raman experiments on silicon-based structures.