Removal of organic micropollutants (OMPs) in the wastewater treatment is greatly important due to their adverse effects on human health and ecosystem. In this work, we provide a new perspective to prepare graphene oxide (GO) nanofiltration (NF) membrane with narrow pore size distribution for robust removal of OMPs. Ferric ions (Fe3+) mediated GO nanosheets are firstly used to prepare GO membrane, then the membrane surface is modified by a targeted coating layer consisting of tannic acid-aminopropyltriethoxysilane (TA-APTES) via their strong affinity to Fe3+, where the larger membrane defects with more Fe3+ would be patched by thicker TA-APTES. Such “speckled” TA-APTES coating can simultaneously enhance antifouling ability and regulate nanochannels of the GO membrane. The resulted GO membrane shows high and steady rejections on various OMPs, even in the long-term operation, cross-flow filtration or under high-pressure. This work proposes an innovative idea for constructing hydrophilic surface and narrow pore size distribution of NF membrane.