In this work, we compare the applicability of three electron–water molecule pseudopotentials in modeling the physical properties of hydrated electrons. Quantum model calculations illustrate that the recently suggested Larsen–Glover–Schwartz (LGS) model and its modified m-LGS version have a too-attractive potential in the vicinity of the oxygen. As a result, LGS models predict a noncavity hydrated electron structure in clusters at room temperature, as seen from mixed one-electron quantum–classical molecular dynamics simulations of water cluster anions, with the electron localizing exclusively in the interior of the clusters. Comparative calculations using the cavity-preferring Turi–Borgis (TB) model predict interior-state and surface-state cluster isomers. The computed associated physical properties are also analyzed and compared to available experimental data. We find that the LGS and m-LGS potentials provide results that appear to be inconsistent with the size dependence of the experimental data. The simulated TB tendencies are qualitatively correct. Furthermore, ab initio calculations on static LGS noncavity structures indicate weak stabilization of the excess electron in regions where the LGS potential preferably and strongly binds the electron. TB calculations give stabilization energies that are in line with the ab initio results. In conclusion, we observe that the cavity-preferring pseudopotential model predicts cluster physical properties in better agreement with experimental data and ab initio calculations than the models predicting noncavity structures for the hydrated electron.