The textile industry is currently under pressure to decrease environmental load related to both the manufacture and the use of textiles. Material recycling may be one of many ways to accomplish such a decrease. Age-induced property changes in cotton textiles are important to understand in order to facilitate the recycling of cotton textiles. Consequently, this study investigates ultrastructural and chemical changes that take place in the cellulose of cotton sheets over a long time period of use and laundering. Ultrastructural changes were studied using water retention value (WRV), specific surface area measurement, scanning electron microscopy and solid state NMR spectroscopy. Chemical changes through
measurement of intrinsic viscosity with and without reductive treatment, molecular mass distribution and carboxylate group content. A substantial decrease in mass average molecular mass from 1,320 to 151 kDa was observed when subjecting the sheets to more than 50 launderings. In contrast, only small differences in WRV, in fibril dimensions and crystallinity estimated using solid state NMR spectra, were observed between sheets laundered 2–4 times and more than 50 times. On one hand, the combination of minor laundering effects of WRV and solid state NMR spectra, together with the large decrease in molecular mass are positive indications for the possibility of recycling cotton into regenerated cellulosic fibres. On the other hand, results show that the specific surface area decreased, which implies that the reactivity of cotton cellulose may decrease during long-term use and laundering.