Novel photoresponsive nanogels were prepared by the self-assembly of spiropyrane-bearing pullulan (SpP).The solution properties of the nanogels could be controlled by photostimulation via isomerization betweenhydrophobic spiropyrane and hydrophilic merocyanine. The molecular chaperone-like activity of the nanogelsin protein refolding was investigated. The activity of citrate synthase significantly increased when theamphiphilicity of SpP nanogels was switched by photostimulation.