Aqueous rechargeable zinc ion batteries are very attractive in large-scale storage applications, because they have high safety, low cost and good durability. Nonetheless, their advancements are hindered by a dearth of positive host materials (cathode) due to sluggish diffusion of Zn2+ in the solid inorganic frameworks. Here, we report a novel organic electrode material of poly 3,4,9,10-perylentetracarboxylic dianhydride (PPTCDA)/graphene aerogel (GA). The 3D interconnected porous architecture synthesized through a simple solvothermal reaction, where the PPTCDA is homogenously embedded in the GA nanosheets. The self-assembly of PPTCDA/GA coin-type cell will not only significantly improve the durability and extend lifetime of the devices, but also reduce the electronic waste and economic cost. The self-assembled structure does not require the auxiliary electrode and conductive agent to prepare the electrode material, which is a simple method for preparing the coin-type cell and a foundation for the next large-scale production. The PPTCDA/GA delivers a high capacity of ≥200 mAh g–1 with the voltage of 0.0∼1.5 V. After 300 cycles, the capacity retention rate still close to 100%. The discussion on the mechanism of Zn2+intercalation/deintercalation in the PPTCDA/GA electrode is explored by Fourier transform infrared spectrometer (FT-IR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) characterizations. The morphology and structure of PPTCDA/GA are examined by scanning electron microscopy (SEM) and transmission electron microscopy (TEM).