Qiongxuan Fan, Jiahao Mei, Tian Li, Chuanlong Zang, Mengjiao Li, Jing Tang, You Xu, Ge Yu, Dandan Liu, Kai Chen, Bing Yang, Jing Huang, Ting Zhou, Bobo Dang
Covalent protein drugs offer therapeutic potential but are limited by slow target engagement and the absence of high-throughput selection platforms. Rapid covalent binding requires coordinated optimization of affinity, stability, and warhead geometry, which is an intrinsically multidimensional challenge. We developed a yeast display platform coupled with chemoselective modification that enables selection of fast-acting covalent proteins without increasing intrinsic warhead reactivity. Using this system, we engineered a covalent programmed death-ligand 1 (PD-L1) antagonistic nanobody with rapid cross-linking kinetics [observed rate constant ( k obs ) = 0.18 min −1 , half-life ( t 1/2 ) = 3.8 min] and improved tumor suppression compared with envafolimab and atezolizumab. Similarly, we engineered a fast-acting covalent interleukin-18 ( k obs = 0.54 min −1 , t 1/2 = 1.3 min) and a covalent miniprotein targeting the receptor binding domain of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), demonstrating applicability across protein modalities.