For exploiting the multifunctional ecological cotton textile products and developing the green modified technology for cotton fabrics, a novel cotton fabric with aloe extract crosslinking was prepared using citric acid as a crosslink agent under the pad-dry-cure procedure. Scanning electron microscopic photographs showed that the modification with aloe extract occurred on the surface of cotton fabric. FT-IR spectra of the modified fabric illuminated that aloe extract crosslinked with cotton fabric through the bridge linkage of citric acid after a series of reaction. The wide angle X-ray diffraction analysis indicated that the crystallinity of aloe extract modified cotton fabric slightly decreased. Furthermore, the changes in the aggregating structure and crystallinity were also reflected in the mechanical property studies of these modified fabrics. After treatment by aloe extract, the breaking strength and elongation of cotton fabric decreased. However, the moisture regain of the modified cotton fabric increased. The results obtained are useful in explaining structure-property correlations with respect to the aggregating structure and crystallinity, and suggest valuable information in planning applications for the aloe extract modified cotton textile products.