1352 wileyonlinelibrary.com maintain the integrity of network structures and mechanical properties of bulk gels, leading to their long-term use with stable functionality. [9][10][11][12][13] The scientifi c community nowadays focus on two major approaches, based on dynamic covalent bond [14][15][16][17] and noncovalent bond, [18][19][20][21][22][23][24][25][26][27][28] to design self-healing hydrogels. Dynamic covalent bond integrates both the stability of covalent bond and the reversibility of noncovalent bond in one system. [ 29 ] These dynamic covalent bonds can build an intrinsic dynamic equilibrium of bond generation and dissociation in hydrogel networks, endowing self-healing performance to the hydrogels. Despite a few examples of self-healing hydrogels based on the dynamic covalent bonds (e.g., phenylboronate esters, [30][31][32] acylhydrazone bonds, [ 29,33 ] disulfi de bonds, [34][35][36] and Diels-Alder reactions, [ 37,38 ] the diffi culty of manipulating in vivo due to their nonautonomous self-healing characteristics, impedes their applications. For instance, selfhealing hydrogel based on dynamically restructuring of phenylboronic esters needs an acid environment (pH 4.2), [ 30 ] while hydrogel based on dynamic disulfi de bonds usually needs an alkali environment (pH 9), [ 34 ] to trigger the corresponding healing process. Moreover, complicated synthetic procedures and unconfi rmed biocompatibility of these self-healing hydrogels may limit their applications. For instance, the self-healing A novel biocompatible polysaccharide-based self-healing hydrogel, CEC-l-OSA-l-ADH hydrogel ("l" means "linked-by"), is developed by exploiting the dynamic reaction of N -carboxyethyl chitosan (CEC) and adipic acid dihydrazide (ADH) with oxidized sodium alginate (OSA). The self-healing ability, as demonstrated by rheological recovery, macroscopic observation, and beam-shaped strain compression measurement, is attributed to the coexistence of dynamic imine and acylhydrazone bonds in the hydrogel networks. The CEC-l-OSA-l-ADH hydrogel shows excellent self-healing ability under physiological conditions with a high healing effi ciency (up to 95%) without need for any external stimuli. In addition, the CEC-l-OSA-l-ADH hydrogel exhibits good cytocompatibility and cell release as demonstrated by threedimensional cell encapsulation. With these superior properties, the developed hydrogel holds great potential for applications in various biomedical fi elds, e.g., as cell or drug delivery carriers.