The main component of phosphogypsum (PG) is CaSO4·2H2O. PG contains a few impurities, heavy metals, and radioisotopes, which limit the use of PG and pose a danger to the environment. In this study, under the excitation of a sodium hydroxide solution, the rheological properties of a paste with granulated blast-furnace slag (GGBS) and PG treated with ultrasonic water washing were investigated. Experimental results showed that the ratio of GGBS to PG and the amount of sodium hydroxide solution significantly affect the density and viscosity of the paste, but the effect patterns of both are different. The maximum viscosity was 498 mPa·s when the ratio of GGBS to PG was 4:1. When the ratio changed from 3:2 to 1:4, the viscosity of the paste gradually decreased by 15.5%, 32.1%, 36.1%, and 46.8%, respectively. In contrast, the ratio of GGBS to PG had a greater effect on the viscosity than the amount of sodium hydroxide solution in terms of the standard consistency water consumption, viscosity, and water release ratio. The larger the PG ratio, the smaller the density, viscosity, and water release ratio of the paste. The variation in the ratio of GGBS to PG had a significant effect on the water film thickness of the paste, demonstrating that the larger the PG mixture, the larger the water film thickness of the paste, which reached 1.122 μm, 2.31 times the minimum water film thickness of the paste. At the same time, the water film thickness of the paste was negatively correlated with the water consumption of the standard consistency, viscosity, and water release ratio, and was positively correlated with the fluidity.