Smart hydrogels have received increasing attention for many applications. Here, we synthesized a class of cationic peptide amphiphiles that can self-assemble into hydrogels by ring-opening polymerization (ROP) and post modification strategy. The incorporation of cationic lysine residues suppresses the formation of fibril-like structure and further the gelation ability of the samples. Sodium alginate (SA) is used to enhance the rheology performance of the hydrogels. The hydrogels exhibit pH-dependent self-assembly and the gelation behavior that enables them to be ideal smart hydrogel systems for biomedical applications. Furthermore, the as-prepared hybrid peptide hydrogels show antibacterial activity.