We report measurements of long-period P wave polarization (P pol) in Australia and Tahiti made by combining modeling of the polarization deviation and harmonic analysis. The analysis of the deviation of the horizontal polarization of the P wave as a function of event back azimuth may be used to obtain information about (1) sensor misorientation, (2) dipping discontinuities, (3) seismic anisotropy, and (4) velocity heterogeneities beneath a seismic station. The results from harmonic analysis and a grid search using Snell's law suggest the presence of a dipping seismic discontinuity beneath stations CTAO and CAN in Australia. These results are consistent with published receiver function studies for these stations. The P pol fast axis orientation is close to the N–S absolute plate motion direction at station TAU (Tasmania), which may be due to plate-motion-driven alignment of olivine crystals in the asthenosphere. Interestingly, measurements of SKS splitting at Tahiti (French Polynesia) show an apparent isotropy, whereas an inversion of P pol observations at PPTL seismic station located in Tahiti suggests the presence of two anisotropic layers. The fast axis azimuth is oriented E–W in the upper layer, and it is close to the NW–SE orientation in the lower layer. Since P pol orientations are used for real-time earthquake locations, especially in poorly instrumented areas such as the South Pacific, we show that the bias from anisotropy and sensor misorientation determined here can be corrected to improve the location accuracy, which yields fundamental data for rapid location necessary for effective tsunami warning.