A new method of coating and surface hydrophobic modification was proposed to treat artificial aggregate aiming at solving the problems of loose and porous surface of artificial aggregate and insufficient binding with cement paste in concrete. Different mass fractions of silane coupling agent solution and silicone resin were used to modify the artificial aggregate of carbonation curing. The effects of modification methods on the water absorption rate, particle strength of artificial aggregate and bond strength of aggregate-cement mortar were studied, and the microstructure of artificial aggregate and the interface morphology between artificial aggregate and cement mortar before and after modification were characterized by meso/micro test analysis methods. The results show that compared with the single use of chemical solution to modify artificial aggregate, the combined modification method significantly optimizes the surface microstructure of artificial aggregate and improves the aggregate performance, and the water absorption rate of aggregate is reduced to 1.74%. When the mass fraction of silane coupling agent is 5%, a modified layer with appropriate thickness is formed on the surface of artificial aggregate, and the binding property between artificial aggregate and cement mortar is significantly improved.