Polyaniline (PANI) nanospheres, nanofibers, and nanoplates were prepared using the oxidative polymerization method. Scanning electron microscopy (SEM) was used to observe the three morphologies of PANI, and their structure was tested using infrared spectroscopy, X-ray diffraction, Raman spectroscopy, and X-ray photoelectron spectroscopy. The influence of particle morphology on the electrorheological (ER) effect was studied through rheological experiments and molecular dynamics (MD) simulation. The experimental and simulation results indicate that without applying an electric field, the nanofibers easily form a three-dimensional network structure in the suspension, resulting in yield stress. The three-dimensional network structure of the nanoplate suspension becomes weaker and the PANI nanosphere suspension lacks the ability to form a three-dimensional network structure. After applying an electric field, under the same condition, the yield stress and electric field-induced shear stress increment of PANI nanofibers are the highest, followed by nanoplates, and those of PANI nanospheres are the lowest. This indicates that the ER effect increases with the increase in particle morphology anisotropy. Through three-dimensional visual simulation analysis, it can be concluded that the enhanced ER effect associated with increased particle anisotropy can be attributed to improved stability in the ER chain structure.