ABSTRACT This study aimed to enhance the antibacterial and biocompatible properties of PLA nonwoven materials by plasma‐assisted surface decoration with selenium nanoparticles. PLA nonwoven materials were pretreated by plasma surface modification technology for varying durations. Subsequently, Se nanoparticles obtained from the redox reaction of sodium selenite were loaded onto the PLA surfaces through impregnation. SEM images demonstrated that plasma pretreatment enhances the uniformity of Se nanoparticles as well as the contents loaded onto the PLA nonwoven materials. Based on EDS analysis, the relative concentration of Se elements increased with longer plasma pretreatment durations, reaching 6.38% after 6 min of treatment. XPS analysis confirmed the presence of elemental selenium nanoparticles. Furthermore, the results of surface wettability showed that the surface of Se/PLA composites changed from hydrophobic to super hydrophilic after the plasma and Se combined treatment. Moreover, bacterial inhibition of the Se/PLA composites substantially improved with increasing plasma pretreatment time. The Se/PLA composites with 6 min of plasma pretreatment showed the best antibacterial performance and biocompatibility, with inhibition rates against Staphylococcus aureus and Escherichia coli reaching 95.75% and 75.54%, respectively, and cell viability was over 99% for L929 cells. These functionalized Se/PLA composites exhibit tremendous potential for applications in novel antibacterial materials.