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Tapioca is economical crop grown in Thailand and continues to be one of the major sources of starch. Nowadays, tapioca starch has been widely used in industrial applications, however the native form of starch has limited the applications. Thus scientists try to modify the properties of starch for increasing the stability of the granules, pastes to low pH, heat, and shear during the food process. We modify the tapioca starch by plasma treatment under an argon atmosphere. The degree of modification is determined by following water content in the starch granules. The tablet samples of native starch are also prepared and compared with the plasma treated starch. Before plasma treatment, the starch tablets are stored under three different relative humilities (RH) including 11%, 68%, and 78%RH, respectively. The samples are characterized using FTIR spectroscopy associated with the degree of cross-linking. The results show that the water molecules are engulfed into the starch structure in two ways, a tight bond and a weak absorption of water molecules which is represented at two wave number of 1630 cm−1 and 3272 cm−1, respectively. The degree of cross-linking can be identified from the relative intensity of these two peaks with the C—O—H peak at 993 cm−1. The results show that the degree of cross-linking increase in the plasma treated starch. The degree of cross-linking of the treated starch with high relative humidity is less than that of the treated starch with low relative humidity.