Improving the development of high-value multifunctional wool fabrics was essential to satisfy diverse needs. Considering the various characteristics of chitosan macromolecules, herein, a padding-cross-linking process was adopted and then multifunctional wool fabrics with outstanding printing effects, shrink resistance, and antibacterial properties were fabricated. The test results showed that chitosan macromolecules loaded successfully on the wool fiber surface by Schiff base reaction. Wool fabrics changed from hydrophobic to hydrophilic due to the existence of chitosan macromolecules. The color strength (K/S value) of the reactive dye inkjet-printed wool fabric was greatly increased from 20.48 to 26.6. The area shrinkage of final samples was 2.53%, which was exceedingly lower than that of the original wool (10.96%). Moreover, the chitosan macromolecules with reactive amino groups endowed wool fabrics with certain antibacterial properties against E. coli and S. aureus. Generally, this study provided guidance for manufacturing multifunctional digital inkjet-printed wool products in mass production.