Metal−organic frameworks (MOFs), MIL-125 and UiO-66, were modified on the butterfly wings (BWs) by chemical bonds, and CdS was grown in situ on them through a solvothermal approach. The BWs enable the biocomposites to possess a wider (>600 nm) and stronger light absorption. The in situ growth method can produce highly active and stable biocomposites. These novel morphologic MOF/CdS biocomposites were characterized using scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and so on. The resulting composites were tested for photocatalytic hydrogen production through water splitting with platinum and lactic acid as the co-catalyst and sacrificial agent, respectively. The two samples showed higher activity than bulk CdS, MOFs, or their composites. Therefore, this paper provides an appropriate method to obtain the MOF/CdS biocomposites, and the resulting biocomposites are proved to be efficient catalyst systems for hydrogen evolution from water under visible light with a wider wavelength.