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Highly efficient removal of bilirubin from blood by hemoperfusion for liver failure therapy remains a challenge in the clinical field due to the low adsorption capacity and slow adsorption kinetics of currently used bilirubin adsorbents (e.g., activated carbon and ion‐exchange resin). Recently, porous aromatic frameworks (PAFs) with high surface areas, tunable structures, and remarkable stability provide numerous possibilities to obtain satisfying adsorbents. Here, a cationic PAF with more mesopores, named iPAF‐6, is successfully constructed via a de novo synthetic strategy for bilirubin removal. The prepared iPAF‐6 exhibits a record‐high adsorption capacity of 1249 mg g−1 and can adsorb bilirubin from 150 mg L−1 to normal concentration in just 5 min. Moreover, iPAF‐6 shows a removal efficiency of 96% toward bilirubin in the presence of 50 g L−1 bovine serum albumin. It is demonstrated that positively charged aromatic frameworks and large pore size make a significant contribution to its excellent adsorption ability. More notably, iPAF‐6/polyethersulfone composite fibers or beads are fabricated for practical hemoperfusion adsorption, which also show better removal performance than commercial adsorbents. This work can offer a new possibility for designing PAF‐based bilirubin adsorbents with an appealing application prospect. [ABSTRACT FROM AUTHOR]