A facile and sustainable synthetic strategy based on the coordination of natural polyphenols with metal ions is developed for the textural engineering of mesocrystals and hierarchical carbon nanomaterials. The desired control of coordination between ellagic acid and zinc ions enables the macroscopic self-assembly behavior of crystalline nanoplatelets to be tailored into round and elongated peanut-like micron-sized mesostructured particles. Direct carbonization of these mesocrystals generates hierarchically porous carbon particles in good yields, possessing bimodal micro- and mesoporous architecture along with a well-preserved macroscopic structure. The pore system provides both small storage sites, demonstrated by high CO2 uptake, and transport channels also accessible by larger molecules.