Reversible light-responsive nanogels were constructed from an amphiphilic spiropyrane-modified pullulan (SpP). The polymer was synthesized by modifying a biodegradable pullulan with carboxyl-containing spiropyrane (Sp) molecules. The SpP structure was confirmed by the appearance of a carbonyl signal in the FT-IR and 1H NMR spectra. The nanogels can be controlled by photostimulation, which results in the reversible structural transformation of the hydrophobic Sp to the hydrophilic merocyanine. The physical properties of the nanogels were confirmed to change dramatically after being irradiated with different wavelengths of light. Drug delivery tests showed that the model drug pyrene was completely captured by the nanogels and then released from the SpP nanogels in a light-dependent manner. This study provides an alternative approach to constructing light-responsive nanocarriers with excellent biocompatibility for drug uptake and release. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40288.