The enhancement of the surface potential of tris(8-quinolinato)aluminum (Alq3) film deposited on ultraviolet (UV)/ozone-treated gold electrodes was confirmed by surface potential measurement, and the ordering of molecular dipoles was suggested. The enhanced surface potential of the order of 10 V decayed rapidly by photoirradiation, due to molecular dipole disordering, but a surface potential of 100–400 mV remained. Interestingly, this remaining surface potential of Alq3 on the UV/ozone-treated gold electrode was always smaller than that of Alq3 film on an untreated gold electrode. It was concluded that the UV/ozone treatment is effective in decreasing the density of surface states at the Alq3-metal interface as well as for the enhancement of molecular dipole ordering.