The water in lunar materials can promote the evolution of lunar geology and environment and provide the necessary conditions for the utilization of lunar resource. Owing to the low resolution of lunar remote sensing methods, it is difficult to obtain direct evidence of water / ice or determine its form of occurrence. Laser Raman spectroscopy can obtain fingerprint information of minerals and water bodies without the need for illumination, sample pretreatment, and non-destructive, providing direct and favorable information regarding the type, distribution range, and content of lunar materials. In this study, Raman spectroscopy was used to detect the water-containing characteristics of typical lunar rocks/minerals and forms such as adsorbed water, ice, crystalline water, and hydroxyl-structured water, and quantitatively analyze the water content. First, a 532 nm laser micro-Raman spectroscopy was used to identify and analyze the water-containing signals of typical lunar minerals and various forms of water in lunar soil simulants. Second, the detection limits of adsorbed water, crystalline water, and hydroxyl-structured water in lunar soil simulants were examined and analyzed, along with the patterns between their content and signal intensity. Finaly, linear regression (LR), ridge regression (RR), and partial least squares regression (PLSR) were employed for quantitatively analyze of the contents of three forms of water in the lunar soil simulants. The results show that (1) the characteristic spectral peaks of the four forms of water in the lunar soil simulants can be clearly identified. The peak distribution regions of the lunar soil simulants components and water bodies are located at 100-1700 cm-1 and 2600-3900 cm-1, respectively. The characteristic spectral peaks of water are manifested as a combination of broad envelope peaks of hydrogen-bonded OH and sharp peaks of non-hydrogen-bonded OH stretching vibrations in varying proportions. (2) Detection limits of adsorbed water, crystalline water (MgSO4·7H2O), and hydroxyl water (Al2Si2O5(OH)4) in the lunar soil simulants are 1.3 wt%, 0.8 wt%, and 0.3 wt%, respectively. (3) A linear relationship exists between the intensity of water-containing peaks and the water content in the lunar soil simulants, with root mean square errors of 1.75 wt%, 1.16 wt%, and 1.19 wt% obtained through LR, RR, and PLSR.