Granite residual soil (GRS) has prominent disintegration characteristics which have induced various geological disasters and engineering problems. The initial moisture content is believed to affect the disintegration of GRS significantly. To explore the effects of the initial moisture content on the soil disintegration characteristics and disintegration mechanism, disintegration tests were performed on remolded GRS with different initial moisture contents via the balance method, and the quantitative disintegration indices were corrected, considering the effects of water-absorption weight gain, in combination with a parallel water-absorption test. The disintegration characteristics and mechanism were thoroughly investigated, starting with the disintegration process curves and disintegration morphology, and combined with strength theory, X-ray diffraction (XRD) and X-ray fluorescence (XRF), the matric suction test, and the triaxial shear test. The results are as follows. (1) The corrected method improves the accuracy of the quantitative disintegration evaluation. (2) During the two disintegration stages, the forms of disintegration are dispersive fragmentation and progressive or block separation, and the soil matric suction and weakening of intergranular joining forces, respectively, are the drivers of disintegration. The first stage is usually completed within 1.5–2 min, and the disintegration ratio is usually within 20%. (3) The trends of change within the disintegration during the two stages show opposite water-content-dependent modes, and the soil samples with lower moisture contents have better water stability and slower disintegration in the second stage. The average disintegration rate of the soil with a moisture content of 24.4% in the first and second stages was approximately 1/5 and 13 times, respectively, that of the soil with a moisture content of 6.1%; these values can be rendered as 0.049%/s and 0.82%/s, respectively. The results provide some theoretical references for soil and water conservation and engineering applications in the GRS field.