The vertical distribution of aerosols governs their interactions with solar radiation and clouds, making it a key factor in their climatic and environmental effects. Existing passive methods for retrieving aerosol layer height (ALH) largely rely on a single observational dimension, such as spectral or multi-angle information, which provides limited constraints under complex aerosol conditions. To address this, we extend conventional spectral approaches by incorporating multi-angle polarimetric observations. Leveraging the high sensitivity of polarization signals to differences between molecular Rayleigh and aerosol scattering, along with broader scattering angle sampling, sensitivity to aerosol vertical structure is significantly enhanced. Using a vector radiative transfer model and information content analysis, we evaluate the contributions of multi-angle and polarimetric information to ALH retrieval. Results show that, compared with radiance-only observations, multi-angle polarimetric measurements substantially increase the degrees of freedom for signal, thereby improving ALH accuracy. An optimal estimation method is developed using HARP2 multi-angle polarimetric observations aboard PACE. Retrieved ALH values are validated against ATLID lidar observations on EarthCARE. For all collocated samples, HARP2 retrievals achieve a root mean square error (RMSE) of 1.03 km, significantly lower than the 1.40 km from TROPOMI, with a near-zero bias (−0.07 km). For smoke, the RMSE is 1.12 km, and for dust it further decreases to 0.92 km. In a typical dust transport event, 84.5 % of retrieval errors are smaller than 1 km, highlighting the marked accuracy advantage of multi-angle polarimetric observations in ALH retrieval.