Organic active materials are regarded as a promising candidate to replace inorganic counterparts owing to their tunable redox activity, mild synthesis condition, and multi-electron reactions. However, these organic materials are limited by their dissolution in the aqueous electrolyte and low electrical conductivity. Herein, we synthesized self-assembled nanorods of perylene-3,4,9,10-tetracarboxylic dianhydride (NRPTCDA) grown on carbon cloth for high-performance Zn-ion storage. The vertical orientation and length of nanorods were controlled through optimizing the synthesis condition, which can facilitate Zn-ion insertion−deinsertion. For an aqueous Zn-ion battery, the NRPTCDA cathode achieved a high capacity of 127.5 mAh g −1 at a current density of 1 A g −1 , which retained 82.10 mAh g −1 even at a high current rate of 50 A g −1 . Additionally, structure-controlled NRPTCDA exhibited 90.1% of rate capability at 100 mV s −1 and 78.91% capacity retention over 10 000 galvanostatic charge−discharge cycles at 10 A g −1 of current density. Additionally, ex situ Xray diffraction, attenuated total reflectance−Fourier transform infrared spectroscopy, and field emission scanning electron microscopy measurements were performed and confirmed structural, chemical, and morphological stability and reversibility of NRPTCDA electrodes for Zn 2+ ion storage.