The development of flexible and wearable healthcare devices facilitates a real-time monitoring of body activities as well as detecting various biosignals, which provided useful information to manage one's health condition for personal health monitoring.

Origami utilizes orchestrated transformation of soft 2D structures into complex 3D architectures, mimicking shapes and functions found in nature. In contrast to origami in nature, synthetic origami lacks the ability to monitor the environment and correspondingly adjust its behavior. Here, magnetic origami actuators with capabilities to sense their orientation and displacement as well as detect their own magnetization state and readiness for supervised folding are designed, fabricated, and demonstrated. These origami actuators integrate photothermal heating and magnetic actuation by using composite thin films (≈60 µm thick) of shape‐memory polymers with embedded magnetic NdFeB microparticles. Mechanically compliant magnetic field sensors, known as magnetosensitive electronic skins, are laminated on the surface of the soft actuators. These ultrathin actuators accomplish sequential folding and recovery, with hinge locations programmed on the fly. Endowing mechanically active smart materials with cognition is an important step toward realizing intelligent, stimuli‐responsive structures.

Magnetic anisotropy in sensors and actuators enables remote and high-degree-of-freedom manipulation of soft robots, as well as cutting-edge control through sensor-actuator feedback systems.

Polymer nanocomposites incorporating inorganic nanofillers have emerged as highly promising electromagnetic interference (EMI) shielding materials, combining mechanical compliance with robust conductive percolation networks. Carbon nanotubes (CNTs) are particularly attractive as conductive fillers because their high aspect ratio facilitates percolation at low loadings. Also, CNTs offer superior mechanical durability under deformation compared to rigid, fracture-prone metal nanowires. For EMI shielding, high electrical conductivity is critical as it enhances both reflection and absorption through efficient charge dissipation and conduction losses. However, achieving highly aligned conductive pathways without degrading the intrinsic electrical properties of CNTs remains a significant challenge. Here, we demonstrate a non-destructive magnetic surface-functionalization and alignment strategy. Using a polydopamine (PDA)-mediated route, pristine multiwalled CNTs are uniformly decorated with Fe3O4 nanoparticles (FMWCNTs). This enables highly effective magnetic field-driven alignment at fields as low as 10 mT, promoting the strategic formation of percolation networks. By optimizing the Fe₃O₄/MWCNT ratio for high saturation magnetization and uniform coverage, the aligned FMWCNTs exhibit significant electrical anisotropy, delivering a 10.7-fold higher electrical conductivity in the parallel configuration compared to the vertical configuration. These findings present a scalable, room-temperature platform for engineering directionally enhanced conductivity in polymer nanocomposites, with broad applicability in advanced EMI shielding, flexible electronics, and advanced packaging technologies.

In article number 2005521, Denys Makarov and co‐workers demonstrate skin‐compliant, stretchable, and printable giant magnetoresistive sensors that can operate in low magnetic fields of 1 mT under extreme mechanical deformations of bending radii of up to 16 μm and 100% stretching. They highlight the application potential of these devices in augmented reality settings, with a sensor‐functionalized finger conducting remote and touchless control of virtual objects.

All‐inorganic CsPbI ₃ perovskite nanocrystals (PNCs) have emerged as promising emitters for optoelectronic applications owing to their high color purity, tunable bandgap, and high photoluminescence quantum yield (PLQY). However, dynamic surface ligands, abundant trap states, and rapid halide ion migration limit their emission efficiency and operational stability. Here, methylammonium (MA ⁺ ), formamidinium (FA ⁺ ), and guanidinium (GA ⁺ ) were systematically investigated as surface modulators for PNCs via an anti‐solvent‐assisted post‐treatment strategy. Spectroscopic analyses and density functional theory calculations reveal that the passivation efficacy is determined by the strength and denticity of hydrogen‐bonding interactions between the organic cations and the PNC surface. Among the three candidates, GA ⁺ exhibits the highest efficacy owing to its trifunctional N─H groups, which enable robust multidentate surface interactions that suppress trap formation and halide ion migration. As a result, GA‐treated PNCs achieve a PLQY of 99.3% and retain ∼80% of their initial PLQY after 9 days under ambient conditions. The resulting perovskite light‐emitting diodes deliver a maximum external quantum efficiency of 10.2% and a maximum luminance of 473 cd m ⁻² , representing a significant improvement over pristine devices. These findings identify molecular hydrogen‐bonding geometry as a key design parameter for surface engineering of efficient and stable PNC‐based optoelectronic devices.