Permanent magnets are essential components for many biomedical systems and electromechanical devices, which may be made into flexible formats to achieve wearable monitoring and effective integration with biological tissues. However, the development of high‐performance flexible permanent magnets is challenging due to their ultrathin geometries, which contradict with the thickness‐dependent magnetic properties. In addition, magnetic membranes with controllable sequences of polarities are difficult to achieve. Here, origami techniques to achieve flexible permanent magnetic membranes with enhanced magnetic field strength and programmable sequences of polarities are presented. Linear Halbach arrays, circular Halbach arrays, and concentric magnets with thicknesses ranging from 130 to 500 µm and bending curvatures ranging from 0.039 to 0.0043 µm−1 are achieved through different folding mechanisms. The origami membranes offer a maximum field intensity of 72 mT and extremely strong magnetic force of 0.21 N cm−2, allowing various novel applications demonstrated through electronics interfacing, cell manipulations, and soft robotics. The origami techniques offer large magnetism and complex spatial field distribution, and enable practical use of thin flexible magnetic membranes in constructing miniaturized or even flexible electromechanical systems and biomedical instruments for magnetic resonance imaging, targeted drug delivery, health monitoring, and cancer therapy.

Deformation of flexible electronics can lead to reconfigurable electrical properties, controllable deployment, and tunable working modes, but approaches to actuate flexible electronics are quite limited. A promising method involves using magnetic fields to yield simple displacement of magnetic membranes. However, realization of complex multiaxial bending and rotations of magnetic membranes remains challenging. Here, flexible origami magnetic membranes with programmable magnetic polarities are used to generate complex spatial deformation through coupling with an external magnetic field and interaction among intrinsic magnetism. The membranes can work as standalone flexible actuators and serve as substrates to trigger spontaneous deformation of the carrying flexible devices such as antennas, energy harvesters, and light‐emitting diode arrays. The membranes can travel on a dry surface or in a liquid environment. They also exhibit the capability to reversibly capture and release objects traveling at 326 mm s–1. Flexible devices on the membranes can offer tunable gains and frequencies as well as novel folding and releasing mechanisms determined by the complex magnetic polarities of the underneath membranes. The origami magnetic membranes can be combined to yield more complicate patterns and magnetic polarities, leading to innovative applications in surgical robots, tunable antennas, and various reconfigurable flexible electronics.

Centrifugal pumps are essential mechanical components for liquid delivery in many biomedical systems whose miniaturization can promote innovative disease treatment approaches. However, centrifugal pumps are predominately constructed by rigid and bulky components. Here, we combine the soft materials and flexible electronics to achieve soft magnetic levitation micropumps (SMLMs) that are only 1.9 to 12.8 grams in weight. The SMLMs that rotate at a rotation speed of 1000 revolutions per min to pump liquids with various viscosities ranging from 1 to 6 centipoise can be used in assisting dialysis, blood circulation, and skin temperature control because of excellent biocompatibility with no organ damage. The development of SMLMs not only demonstrates the possibility to replace rigid rotating structures with soft materials for handling large volumes of fluids but also indicates the potential for fully flexible artificial organs that may revolutionize health care and improve the well-being of patients.