ABSTRACT:A new type of hydrogel, transparent cellulose hydrogel (TCG), is the aqueous dispersion of cellulose nanofibers (microfibrils) 10 nm in width and several hundreds nanometers in extended fiber length, and shows unique rheological properties leading to unique applications. The rheological properties of TCG, especially their dependences on temperature were investigated through the spin-spin relaxation time (T 2 ) analysis in 1 H NMR for water in the systems. Viscosity under low shear stress and T 2 of water (being very short for T 2 value) were proved to be constant in a wide range of temperature (ca. 30-80 C). These results may be explained by two considerations that network in TCG gradually grows with increasing temperature but collapses by adding weak shear stress and that TCG gel has large amount of bound water. It was also confirmed that the ionic strength such as pH and NaCl concentration sensitively influences on rheological parameters. With increasing ionic strength, the network formation and the successive aggregation of microfibrils occur and both should be interpreted in terms of the electrostatic interaction between negative charge on a cellulose surface and cationic aqueous layer around it (i.e., electric double layer). [DOI 10.1295/polymj.36.684] KEY WORDS Cellulose / Hydrogel / Nanofiber / Microfibril / Rheology / Spin-Spin Relaxation Time / Network / We have already found a preparation method of a new type of hydrogel, transparent cellulose hydrogel (TCG, Figure 1a), an aqueous dispersion of cellulose microfibrils (degree of polymerization: ca. 40) having low crystallinity with about 10-15 nm in diameter and several hundred nanometers in extended length ( Figure 1b) and reported the results for its characterization and properties. 1,2 This new nanomaterial was prepared by downsizing by chemical (hydrolysis reaction) 3 and mechanical (smashing by a ultra high pressure homogenizer) techniques. Resultant cellulose microfibrils in TCG are flexible fibrous particles, i.e., ''nanofibers'', having nano-size diameter (Figure 1b) and show strong attractive interaction based on hydrogen bonding between hydroxyl groups localized densely on their surfaces, leading to quite unique rheological properties. In view of the application, four major unique properties of TCG are pointed out 2 as follows: 1) Rheological properties such as very high viscosity under the low share stress, a large thixotropic character and low fluctuation of rheological parameters in the range of ambient temperature to the higher temperature region, 2) Formation of transparent coating film on substrate materials by drying, 3) Formation of cellulose microspheres having average particle size of less than 5 mm by spray drying, and 4) Stabilizing ability as an additive for aqueous suspension systems such as aqueous dispersion of inorganic particles (SiO 2 , TiO 2 , . . ., etc.) and O/W type emulsion (also as an emulsifier).Especially from an industrially applicable aspect, we discovered that TCG is a gel which can be sprayed by only ...