This study investigated, for the first time, the antimicrobial properties of polyethylene glycol-functionalized poly(N-phenylglycine) nanoparticles (PNPG-PEG NPs). PNPG-PEG NPs exhibit high extinction coefficient in the near-infrared (NIR) region; they can convert light energy into heat energy with high thermal transformation efficiency. Additionally, they can generate cytotoxic reactive oxygen species (ROS) upon light irradiation. Also, PNPG-PEG NPs are not cytotoxic. All these properties make them appropriate for combined dual-modal photothermal and photodynamic therapies. The antibacterial activity of PNPG-PEG NPs was assessed using Escherichia coli (Gram-negative) and Staphylococcus aureus (Gram-positive) pathogenic strains. The results revealed that NIR light (810 nm) irradiation for 10 min could kill effectively the planktonic bacteria and destroy Escherichia coli and Staphylococcus aureus biofilms. The results demonstrated that PNPG-PEG NPs represent a very effective nanoplatform for killing of pathogenic bacteria.