Fresh and clean water is highly demanded throughout the world. To effectively address the need, nanomaterials enabled nanotechnology has been explored as a means of more efficient, reliable, and environmentally friendly approach towards water treatment practices. One concern in adopting nanomaterials is how to retrieve them from water body to avoid secondary contamination. In this work, the earth abundant and sustainable wood, e.g., basswood, was selected and carbonized into porous carbon as host skeleton, and metal-organic frameworks (MOFs), e.g., MOF-199 with extremely high surface area, were grown throughout all channels in the porous basswood carbon. Targeting the traditional organic pollutant, methyl orange (MO), the combination of MOFs and basswood carbon (MOFs@carbon) demonstrates a remarkable adsorption capacity, which is 243% and 454% higher than basswood carbon and MOF-199, respectively. Such an outstanding adsorption performance originates from that the positively charged carbon pulls MO molecules close to carbon surface, leading to a high MO molecule concentration, and then the concentration gradient drives the MO molecules to be stored inside MOFs, functioning like pockets. These findings highlight the potential application of coupled MOFs and biomass carbon in addressing water remediation.