Here we report on the fabrication and characterization of temperature-responsive electrospun nanofiber meshes using N-isopropylacrylamide homopolymer (PNIPAAm). The effect of molecular weight on fiber formation and their thermoresponsive shrinking/dissolution behaviors were investigated. The PNIPAAm fiber meshes showed much faster temperature-dependent shrinking or dissolution than that of its corresponding film due to its unique fibrous structure. By utilizing these quick and dynamic shrinking/dissolution properties, we successfully demonstrated the temperature-modulated on-off capture/release systems for macroscopic or mesoscopic-scale objects. Finally, we explored the potential application of PNIPAAm meshes for cell storage.