In the present work, novel cellulose (C)/Antarctic krill protein (AKP) composite fibers with a multiple cross-linking network were prepared using glutaraldehyde (GA) as cross-linking agent to improve the fiber's properties. The structure and properties of fibers were characterized by different techniques including FTIR, NMR, XRD, SAXS, SEM and electronic single yarn strength tester, etc. The results indicate that the reaction of GA with C and AKP separately forms a multiple cross-linking network. The C/AKP composite fibers with a multiple cross-linking network has stronger crystallization ability, higher orientation degree and deeper trench than C/AKP composite fibers. The breaking stress and wet strength of composite fibers reaches the maximum of 1.04 cN/dtex and 0.55 cN/dtex at GA content of 0.2 wt%. And the fatigue and tensile properties, hygroscopicity and moisture retention of C/AKP composite fibers has been improved. The development of C/AKP composite fibers with a multiple cross-linking network could be a promising candidate for biomedicine applications.