swelling and pH-responsivity rather than prompt disintegration. [13,14] To address this issue, one can postcross-link the multilayer film to inhibit the excessive swelling and disintegration. [15,16] This approach, in general, has several shortcomings though: i) the common cross-linkers, e.g., glutaraldehyde, are mostly toxic, ii) the introduced cross-linker could modify the physicochemical properties of the film, iii) additional postcrosslinking and rinsing steps are required, iv) diffusion barrier could cause inhomogeneous cross-linking within the film, and v) controlling the cross-linking density is challenging since it requires changing the concentration of cross-linker, crosslinking time, or cross-linker type.Oxidation of ALG using sodium metaperiodate produces aldehyde groups that can then directly bind to amine groups of CHI through a Schiff base reaction. [17][18][19][20][21] Therefore, oxidized alginate, also known as alginate dialdehyde (ADA), allows for simultaneous cross-linking during the LbL deposition. Accordingly, while the chief driving force for the LbL assembly is the electrostatic attractions, the adsorbed polymer chains upon each deposition step can directly cross-link to the beneath layer. Hence, this approach can provide a more homogenous crosslinked network without the need for hazardous chemicals or rigorous post-treatments. We recently showed that CHI/ADA films fabricated at pH 6 respond to pH changes (acidic and alkaline) in terms of reversible swelling/shrinkage without disintegration up to 6 d. [22] In this work, we demonstrate that we can effectively modulate the swelling capacity and pH-responsiveness of CHI/ADA multilayer films by i) changing the cross-linking density through systematically varying the oxidation degree of ADA and ii) fabricating the films at different pH values. To do so, we prepared CHI/ADA multilayer films at two different pH values (3 and 6) using ADA of different oxidation degrees (0%, 5%, 25%, and 75%). Quartz crystal microbalance with dissipation monitoring (QCM-D) and spectroscopic ellipsometry measurements were simultaneously conducted to monitor the film properties.