Bae, GunhyuJeon, Yoo SangKo, Min JunKim, YuriHan, Seong BeomThangam, RamarKim, WonsikJung, Hee JoonLee, SungkyuChoi, HyojunMin, SunhongHong, HyunsikPark, SangwooKim, Seong YeolPatel, Kapil D.Li, NaShin, Jeong EunPark, Bum ChulPark, Hyeon SuMoon, Jun HwanKim, Yu JinSukumar, Uday KumarSong, Jae JunKim, Soo YoungYu, Seung HoKang, Yun ChanPark, SteveHan, Seung MinKim, Dong HweeLee, Ki BumWei, QiangBian, LimingPaulmurugan, RamasamyKim, Young KeunKang, Heemin2025-05-232025-05-231616-301XORCID:/0000-0002-0393-9166/work/171153415http://www.scopus.com/inward/record.url?scp=85108191250&partnerID=8YFLogxKhttps://hdl.handle.net/1885/733753190Developing materials with the capability of changing their innate features can help to unravel direct interactions between cells and ligand-displaying features. This study demonstrates the grafting of magnetic nanohelices displaying cell-adhesive Arg-Gly-Asp (RGD) ligand partly to a material surface. These enable nanoscale control of rapid winding (“W”) and unwinding (“UW”) of their nongrafted portion, such as directional changes in nanohelix unwinding (lower, middle, and upper directions) by changing the position of a permanent magnet while keeping the ligand-conjugated nanohelix surface area constant. The unwinding (“UW”) setting cytocompatibility facilitates direct integrin recruitment onto the ligand-conjugated nanohelix to mediate the development of paxillin adhesion assemblies of macrophages that stimulate M2 polarization using glass and silicon substrates for in vitro and in vivo settings, respectively, at a single cell level. Real time and in vivo imaging are demonstrated that nanohelices exhibit reversible unwinding, winding, and unwinding settings, which modulate time-resolved adhesion and polarization of macrophages. It is envisaged that this remote, reversible, and cytocompatible control can help to elucidate molecular-level cell–material interactions that modulate regenerative/anti-inflammatory immune responses to implants.G.B. and Y.S.J. contributed equally to this work. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (Ministry of Science and ICT) (No. 2020R1C1C1011038 and 2019R1A2C3006587). This work was also supported by a Korea University Grant. HAADF‐STEM imaging was conducted with the support of the Korea Basic Science Institute. This work made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205), the MRSEC IRG2 program (NSF DMR‐1720139) at the Materials Research Center, the International Institute for Nanotechnology (IIN), the Keck Foundation, and the State of Illinois, through the IIN. All animal studies were carried out after approval by the Institutional Animal Care and Use Committee of Korea University.enPublisher Copyright: © 2021 Wiley-VCH GmbHadhesion assemblymacrophage polarizationnanohelix motionremote manipulationreversible ligand unwinding2021-09-0910.1002/adfm.20210340985108191250