This study investigated the T2 spectrum of hydrogen nuclear magnetic resonance (1H NMR) signals in cement paste with water-to-cement ratios (w/c) of 0.2, 0.35, and 0.5 under three different saturation methods (natural soak, vacuum saturation, and vacuum saturation with high pressure). The saturation degree and pore structure of the cement paste under different saturation methods has been calculated through the linear relationship between water absorption and increment of NMR amplitude intensity. The results showed that the saturation degree of the cement paste increased progressively with the duration of saturation until it reached a state of equilibrium. It can increase saturation degree and reduce the saturation time by increasing the saturation pressure, and vacuum saturation with high pressure is necessary for cement paste with lower w/c. It is important to noted that conditions such as unsaturation, natural soak, and vacuum saturation may result in incomplete water saturation, leading to a partial loss of the 1H NMR signal amplitude intensity and underestimation of porosity measurements. Considering the duration of saturation and the degree of saturation, it is recommended a saturation duration of at least 4 h with a vacuum pressure of 8 MPa for cement paste with w/c ratio of 0.2 and 0.35. For cement paste with w/c of 0.5, a saturation duration of at least 0.5 h with a vacuum pressure of 8 MPa is suggested.