Highly conductive and optical transparent Al doped ZnO (AZO) thin film composing of ZnO with Zn-Al-O interface was fabricated by thermal atomic layer deposition (ALD) method. The as-prepared AZO thin film exhibits excellent electrical and optical properties, with high stability and compatibility with temperature-sensitive flexible photoelectronic devices: film resistivity is as low as 5.7 × 10-4 Ω·cm; the carrier concentration is high up to 2.2 × 1021 cm-3; optical transparency is greater than 80 % in a visible range; the growth temperature is below 150 °C on the PEN substrate. Compared with the conventional AZO film containing by ZnO and Al2O3 interface, we propose that the underlying mechanism of the enhanced electrical conductivity for the current AZO thin film is attributed to the oxygen vacancies deficiency derived from the free competitive growth mode of Zn-O and Al-O bonds in Zn-Al-O interface. The flexible transparent transistor based on this AZO electrode exhibits the favorable threshold voltage and Ion/Ioff ratio, showing promising for use in high resolution, fully transparent and flexible display applications.