The widespread use of chemicals has brought serious water pollution threatening human health and environment, which requires green, fast, and low‐cost purification urgently. Here, we build up a novel material family of sky‐parking‐like 3D structured graphene oxides (SP‐GOs) with adjustable interlayer‐space of 0.8–1.7 nm via the insertion of different sized diamine compounds as support pillars between GO layers. The assembled 3D SP‐GOs exhibit superior adsorption capacity and short removal time for various aromatic organic compounds in water, achieving record‐breaking maximum adsorption capacity of 535.79 mg g−1 toward the most common water‐pollutant bisphenol A (BPA) at ambient conditions as well as significantly improved removal of other organic pollutants including sulfapyridine, carbamazepine, ketoprofen and 2‐naphthol. The construction of SP‐GO provides a simple approach for evolving the GO material from 2D to 3D and a new avenue for the decontamination of pollutants in environmental remediation.