Commercial production of transparent conducting oxide (TCO) polycrystalline films requires high electrical conductivity with minimal degradation in optical transparency. Aqueous solution deposited TCO films would reduce production costs of TCO films but suffer from low electrical mobility, which severely degrades both electrical conductivity and optical transparency in the visible spectrum. Here, we demonstrated that grain boundary modification by ultra-violet laser crystallization (UVLC) of solution deposited aluminium-doped zinc oxide (AZO) nanocrystals results in high Hall mobility, with a corresponding dramatic improvement in AZO electrical conductance. The AZO films after laser irradiation exhibit electrical mobility up to 18.1 cm2 V−1 s−1 with corresponding electrical resistivity and sheet resistances as low as 1 × 10−3 Ω cm and 75 Ω/sq, respectively. The high mobility also enabled a high transmittance (T) of 88%-96% at 550 nm for the UVLC films. In addition, HAZE measurement shows AZO film scattering transmittance as low as 1.8%, which is superior over most other solution deposited transparent electrode alternatives such as silver nanowires. Thus, AZO films produced by the UVLC technique have a combined figure of merit for electrical conductivity, optical transparency, and optical HAZE higher than other solution based deposition techniques and comparable to vacuumed based deposition methods.