The utilization of solar energy to decompose water and produce hydrogen is one of the important strategies to solve the problems of ecological environment and energy crisis. Herein, a series of CdS-modified Metal-Organic Frameworks (MOFs) composites Zn(LFor)-MOF/CdS were successfully prepared through the reaction of N-(4-pyridine-methyl)-l-valine·HCOONa (NaLFor), Zn acetates, and CdS nanoparticles. The composite Zn(LFor)-MOF/CdS exhibit a very high photocatalytic performance for hydrogen production from water cracking under visible light irradiation, which is superior to the pristine MOF and cadmium sulfide materials. The hydrogen production based on different proportions of Zn(LFor)-MOF/CdS materials were investigated, and the prepared Zn(LFor)-MOF/CdS (4:1) material showed excellent hydrogen evolution performance with the hydrogen yield reaching 267.6 μmol/h. Zn(LFor)-MOF/CdS (4:1) has a high photocurrent intensity, which can effectively inhibit the photoelectron-hole recombination, improve the electron-hole transport ability at the interface, accelerate the electron migration, which makes this material a high hydrogen production photocatalytic activity.