Developing simple, yet effective strategies to program cell–cell interactions facilitate the study of fundamental multicellular behavior and the development of cell-based therapeutics. Here we report cell-membrane-anchored DNA nanoplatform for programming cellular interactions. The membrane-anchored framework nucleic acid clustering can be programmed by DNA probabilistic circuits, to modulate the recognition capability of natural killer cells and control their interactions with cancer cells for enhancing efficient cancer cell killing. This work provides insights for precise control over cellular interactions and opens new opportunities for the development of cell-based immunotherapy.