By mimicking certain biochemical and physical attributes of biological cells, bioinspired particles have attracted great attention for potential biomedical applications based on cell-like biological functions. Inspired by leukocytes, hierarchical biointerfaces are designed and prepared based on specifi c molecules-modifi ed leukocyte-inspired particles. These biointerfaces can effi ciently recognize cancer cells from whole blood samples through the synergistic effect of molecular recognition and topographical interaction. Compared to fl at, mono-micro or nano-biointerfaces, these micro/nano hierarchical biointerfaces are better able to promote specifi c recognition interactions, resulting in an enhanced cell-capture effi ciency. It is anticipated that this study may provide promising guidance to develop new bio-inspired hierarchical biointerfaces for biomedical applications.