The mechanism responsible for unusual hygro-mechanical properties of tension wood containing the gelatinous layer (G-layer) was investigated. Tension and normal wood specimens were sampled from the leaning stems of a 75- and a 40-year-old Kunugi oak (Quercus acutissima) tree, and the moisture dependencies of the longitudinal Young's modulus and longitudinal dimensions were measured. The results, which were analyzed in relation to the anatomical properties of the specimens, revealed that the ratio of increase in the longitudinal Young's modulus with drying was higher in the G-layer than in the lignified layer (L-layer); the longitudinal drying shrinkage displayed a similar pattern. It was found that the lattice distance of the [200] plane in the cellulose crystallite increased with drying, moreover, the half-width of the [200] diffraction peak increased with drying, which was remarkable in the tension wood. Those results suggest that in the green state, the polysaccharide matrix in the G-layer behaves like a water-swollen gel; however, it is transformed into a condensed and hard-packed structure by strong surface tension during moisture desorption, which is a form of xero-gelation. However, in the L-layer, condensation and subsequent xero-gelation of the polysaccharide matrix was prevented by the hydrophobic lignin that echanically reinforces the matrix.