Hyaluronic acid (HA) is extensively utilized in biomedical applications, and its functionality can be enhanced by introducing aldehyde groups (─CHO) through oxidation. In this study, cold atmospheric plasma (CAP) was used to treat aqueous HA solutions, resulting in the formation of plasma‐modified HA (PMHA) containing ─CHO groups. The free radicals generated from interactions between water molecules and CAP particles reacted with HA, leading to the oxidation of hydroxyl groups into ─CHO and the cleavage of glycosidic bonds, causing molecular depolymerization. The PMHA was then used to synthesize hydrogels in combination with carboxymethyl chitosan and ɛ‐polylysine. This study presents an effective approach for generating HA with aldehyde functionalities and offers insights into the interaction between CAP and polysaccharides.