The instability in solution and aggregation-induced self-quenching of indocyanine green (ICG) have weakened its fluorescence and photothermal properties, thus inhibiting its application in practice. In this study, the cationic and anionic liposomes containing ICG were prepared based on 1,2-dioleoyl-3-trimethylammonium-propane (DOTAP) and 1,2-dipalmitoyl--glycero-3-phospho-rac-glycerol (DPPG), respectively. Molecular dynamics (MD) simulations demonstrate that ICG molecules are better distributed in the membranes of cationic DOTAP-based liposomes, leading to a superior fluorescence and photothermal performance. The liposomal ICG also shows the physical and photothermal stability during irradiation and long-term storage. On this basis, the prepared DOTAP-based liposomal ICG was encapsulated in the self-healing hydrogel formed by guar gum through the borate/diol interaction. The proposed liposomal ICG-loaded hydrogel can not only convert near-infrared (NIR) light into heat effectively but also repair itself without external assistance, which will realize potent photothermal therapy (PTT) against bacterial infection and provide the possibility for meeting the rapidly growing needs of modern medicine.