Soft Viscoelastic Magnetic Hydrogels from the In Situ Mineralization of Iron Oxide in Metal-Coordinate Polymer Networks

[Image: see text] The design of soft magnetic hydrogels with high concentrations of magnetic particles is complicated by weak retention of the iron oxide particles in the hydrogel scaffold. Here, we propose a design strategy that circumvents this problem through the in situ mineralization of iron oxide nanoparticles within polymer hydrogels functionalized with strongly iron-coordinating nitrocatechol groups. The mineralization process facilitates the synthesis of a high concentration of large iron oxide nanoparticles (up to 57 wt % dry mass per single cycle) in a simple one-step process under ambient conditions. The resulting hydrogels are soft (kPa range) and viscoelastic and exhibit strong magnetic actuation. This strategy offers a pathway for the energy-efficient design of soft, mechanically robust, and magneto-responsive hydrogels for biomedical applications.