Understanding photocurrent conversion of layered double hydroxide (LDH) materials will be a key step in the future application of these materials to light-capturing molecular devices. In the present study, ultrathin nickel-iron layered double hydroxide/dye (NF-LDH/dye) Langmuir-Blodgett (LB) semiconductor films were prepared using an LB device and deposited on an indium tin oxide (ITO) substrate as a photoanode. The photoelectric conversion efficiency of the prepared LB semiconductor film materials was tested. A comparative experiment was performed to effectively explore the photoelectric conversion performances of the LB semiconductor film materials. Specifically, the NF-LDH cast film electrode, the dye cast film electrode, and an ultrathin composite LB film electrode were used as typical samples to explore photoelectric conversion performances. The electrochemical workstation was used to study the photocurrent density, linear scanning voltammetry curve, and electrochemical impedance spectroscopy of LB film electrodes with different layers. The results show that the film electrode cast by LDH alone or dye alone produces weak photocurrent. The photoelectric conversion efficiency of the LB film electrode is enhanced due to the different dyes' molecular structures and/or aggregations on the surface of LDH with various morphological patterns. The combined NF-LDH/dye composite LB film photoelectrode can generate a photocurrent that is 2-5 times stronger than the raw material, and the stable use efficiency is more than 92%. Present obtained composite LB films demonstrated a uniform morphology and good photoelectric conversion ability. This work provides a useful reference for the field of LDH semiconductor optoelectronic devices and solar cells.