In order to settle the problems in the traditional SILAR method for CdS deposition, such as smaller particles and being difficult to enhance the sensitive layers, an improved spin-coating assisted successive ionic layer reaction method (S-SILR) substituted for the traditional SILAR method is used to deposit the CdS nanocrystals. The comparison between the improved and traditional methods is studied after depositing the CdS nanocrystals onto the ZnO nanorod arrays with the two approaches. Different analysis methods, SEM, XRD, UV-vis and the transit photocurrent measurement are conducted to characterize the morphologies and structures of the samples, as well as investigating the light absorption properties, and the photoelectric conversion performance of the electrodes. The results indicate that the CdS nanocrystals photosensitive layers could be totally coated onto the ZnO nanorod arrays more easily by the improved S-SILR method; the light absorption properties and the photoelectric conversion performance of the electrodes prepared by the improved S-SILR method are more excellent compared with those electrodes prepared by the traditional SILAR method. The improvement of the CdS deposition method has certain guiding significance in enhancing the operability of the preparation technology and the photovoltaic performance of the solar cells.