In this paper, microstructured and nanostructured Al2O3-13wt.%TiO2 coatings were prepared on Ti-6Al-4V alloys by plasma spraying and laser remelting. Optical metallographic microscopy (OM), scanning electric microscopy (SEM) and micro-hardness test methods were used to investigate the effects of laser remelting on the microstructure and properties of the coatings. The test results show that the pores and lamella defects of the as-sprayed coatings were eliminated to obtain smooth and dense coatings after laser remelting, and a good metallurgical bonding was formed between the laser-remelted coatings and the substrates. After laser remelting, the average Vickers hardness values of the laser-remelted microstructured and nanostructured Al2O3-13wt.%TiO2 coatings were increased from 803 HV0.3 and 846 HV0.3 to 1 111 HV0.3and 1 451 HV0.3.