Waste shells can be used to treat wastewater, e.g., livestock and poultry wastewater, containing heavy metals. Shells can be crosslinked with organic compounds to synthesize hydrates with improved adsorption efficiency, which is difficult to separate from wastewater. Percolation membrane and composite adsorbent were prepared using PVA and oyster shell as the main materials to construct a membrane-adsorbent coupled system for the treatment of wastewater with heavy metals. During the treatment process with the coupled system, the adsorbent was not in direct contact with wastewater and could be easily separated. Shell-based adsorbents were less prone to clumping and loss with fluent. The removal of heavy metal ions by modified adsorbent material in the dynamic running method was more than 20 times higher than that of unmodified shell material in the static method. This may be attributed to the surface modification, which improved the surface lubricity of the adsorbent material, coupled with the dynamic adsorption method, which avoided the occurrence of agglomeration of the adsorbent material and enhanced the external mass transfer process of heavy metals to modified adsorbents. The coupled system and dynamic running method have potential applications in treating heavy metal contamination in fecal wastewater in remote rural areas.