The aim of this study was to overcome drawbacks of the inhomogeneous dispersion and facile agglomeration of nano-ZnO/poly(N-isopropylacrylamide) composite hydrogels (nano-ZnO/PNIPAm composite hydrogels) during synthesis and improve the anti-mold property of the nano-ZnO/PNIPAm composite hydrogels. Here, nano-ZnO/PNIPAm composite hydrogels were prepared by the radical polymerization method. Fourier transform infrared (FTIR) spectroscopy, transmission electron microscopy (TEM), differential scanning calorimeter (DSC), and dynamic light scattering (DLS) were used to characterize the effects of different dispersants on the particle sizes, dispersions, and phase transition characteristics of the nano-ZnO/PNIPAm composite hydrogels. The anti-mold properties of nano-ZnO/PNIPAm composite hydrogels were studied. Results revealed that the nano-ZnO/PNIPAm composite hydrogel prepared by the addition of nano-ZnO dispersion liquid exhibited the smallest particle size, the most homogeneous dispersion, and the highest stability. The addition of the dispersant did not change the phase transition characteristics of nano-ZnO/PNIPAm, and the nano-ZnO/PNIPAm composite hydrogels (P_f) exhibited good anti-mold properties to the bamboo mold.