In this letter, non-vacuum ultrasonic spray pyrolysis deposition was used to grow Al2O3/TiO2 thin film as the metal–insulator–semiconductor–insulator–metal ultraviolet photodetector (MISIM UV PD). The anatase TiO2 with 400 °C annealing was used as the active layer of the UV PD. X-ray diffraction and Raman spectra were used to characterize the crystal phase of the TiO2. The Al2O3/TiO2 MISIM UV PD has lower dark current ( $\sim 57.2$ pA), higher photoresponse ( $\sim 24.48$ A/W), and higher detectivity ( $\sim 8.25 \,\, \times \,\, 10^{13}$ Jones), all of which were better than the TiO2 MSM UV PD. Similar device performance was obtained from the SiO2/TiO2 MISIM UV PD. The external quantum efficiency of the Al2O3/TiO2 and SiO2/TiO2 MISIM UV PDs was 8204% and 6840%. Such high external quantum efficiency results from the internal photoconductive gain and the interfacial trap controlled charge injection.