If self-healing materials can be prepared via simple technology and methods using nontoxic materials, this would be a great step forward in the creation of environmentally friendly self-healing materials. In this paper, the specific structural parameters of the various hydrogen bonds between chitosan (CS) and polyacrylic acid (PAA) were calculated. Then, multilayer polyelectrolyte films were fabricated with CS and PAA based on layer-by-layer (LbL) self-assemble technology at different pH values. The possible influence of pH on the (CS/PAA)*30 multilayer polyelectrolyte film were investigated. The results show that the interactions between CS and PAA, swelling capacity, microstructure, wettability, and self-healing ability are all governed by the pH of the CS solution. When the pH value of the CS solution is 3.0, the prepared multilayer polyelectrolyte film (CS3.0/PAA2.8)*30 has fine-tuned interactions, a network-like structure, good swelling ability, good hydrophilicity, and excellent self-healing ability. This promises to greatly widen the future applications of environmentally friendly materials and bio-materials.
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