A novel electrosprayed bilayer film composed of an over-layer (L 2) of aluminium-doped ZnO (AZO) nanoflakes (NF-AZO) and a under-layer (L1) of AZO nanocrystallites structure (NC-AZO) named BL:NF/NC-AZO is studied as an excellent field-emitter. The XRD pattern demonstrated that the doped bilayer film has preferential growth along the c-axis with hexagonal wurtzite structure and the (0 0 2) peak shifted toward the larger angle side after doping. The lowest turn-on field of ∼2.8 V μm-1, highest emission current density of 1.95 mA cm-2 is obtained for BL:NF/NC-AZO under the field of 6.8 V μm-1 and as well as the highest field enhancement factor (β) is estimated to be 4370 ± 3, compared to pure ZnO bilayer film (BL:NF/NC-ZnO) and also better than NC-AZO film and possesses the excellent long term stability of emission current. The PL intensity of doped ZnO bilayer film is very much stronger than pure ZnO bilayer structure. The superior field emission properties are attributed to the better morphologies, Al-doping and better crystallinity of bilayer AZO films. © 2014 The Royal Society of Chemistry.