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2D nanomaterials have long been considered for development of high permeability membranes. However, current processes have yet to yield a viable membrane for practical use due to the lack of scalability and substantial performance improvements over existing membranes. Herein, an ultrathin graphene oxide (GO) membrane with a permeability of 1562 mL h−1 mmHg−1 m−2, two orders of magnitude higher than the existing nanofiltration membranes, and a tight molecular weight cut‐off is presented. To build such a membrane, a new process involving self‐assembly and optimization of GO nanoplatelet physicochemical properties is developed. The process produces a highly organized mosaic of nanoplatelets enabling ultra‐high permeability and selectivity. An adjustable molecular interlinker between the layers enables absolute nanometer‐scale size cut‐offs. These characteristics promise significant improvements to many nanoparticle and biological separation applications. In this work, the performance of the membrane in blood dialysis scenarios is evaluated. Urea and cytochrome‐c sieving coefficients of 0.5 and 0.4 are achieved while retaining 99% of albumin. Hemolysis, complement activation, and coagulation studies exhibit a performance on par or superior to the existing dialysis membrane materials. [ABSTRACT FROM AUTHOR]