This study reports on a simple and efficient strategy to prepare macroscopically assembled nanostructured porous carbon (MNPC) based on metal-phenolic interactions. The abundant coordination sites contained in tannic acid enable to form a stable, interconnected hydrogel dough. The porosity evolution mechanism during carbonization process is studied by temperature programmed desorption-mass spectroscopy. Hierarchical pore structure of the MNPC can be developed by modulating the zinc chloride content. The resulting material provides versatile adsorption behaviors for various ranging from small gas molecules to larger molecules such as dye, oil and organic solvents.