Surface states and interfacial phenomena at the undoped polycrystalline semiconductor particale-electrolyte interfaces were qualitatively analyzed based on the zeta potentials which were measured with microelectrophoresis measurements. The suspensions were composed of the undoped polycrystaline silicon(Si) or gallium arsenide (GaAs) semiconductor particles stalline Si and GaAs particles in the KCl electrolytes was 3.73~6.2x10**-4 cmulcornerV.sec and -2.3~1.4x10**-4cmulcornerV.sec at the same conditions, respectively. The range of zeta potentials corresponding to the electrophoretic mobilities is 47.8~80.1mV and -30.1~17.9mV, respectively. The variation of the zeta potentials of the undoped polycrystalline Si was similar to the doped crystalline Si. On the other hand, two points of zeta potential reversal occurred at the undoped polycrystalline GaAs-KCl electrolyte interfaces. The surface states of the undoped polycrystalline Si and GaAs were dominated by positively charged donor surface states. These surface states are attributed to adsorbed ion surface states (slow states) at the semiconductor oxide layer-electrolyte interfaces.