We report a facile and general approach to using generation 2 (G2) poly(amidoamine) (PAMAM) dendrimers for simultaneous stabilization and functionalization of electrospun poly(gamma-glutamic acid) nanofibers (gamma-PGA NFs). In this study, uniform gamma-PGA NFs with a smooth morphology were generated using electrospinning technology. In order to endow the NFs with good water stability, amine-terminated G2.NH2 PAMAM dendrimers were utilized to crosslink the gamma-PGA NFs via 1-ethyl-3-(3-dimethylami-nopropyl) carbodiimide coupling chemistry. Under the optimized crosslinking conditions, G2.NH2 dendrimers partially modified with fluorescein isothiocyanate (Fl) or folic acid (FA) were used to crosslink gamma-PGA NFs. Our results reveal that G2.NH2-Fl is able to simultaneously render the NFs with good water stability and fluorescence property, while G2.NH2-FA is able to simultaneously endow the NFs with water stability and the ability to capture FA receptor-overexpressing cancer cells in vitro via ligand-receptor interaction. With the tunable dendrimer surface chemistry, multifunctional water-stable gamma-PGA-based NFs may be generated via a dendrimer crosslinking approach, thereby providing diverse applications in the areas of biosensing, tissue engineering, drug delivery, and environmental sciences.