Reprogrammable magneto-responsive soft actuators capable of working in enclosed and confined spaces and adapting functions under changing situations are highly demanded for new-generation smart devices. Despite the promising prospect, the realization of versatile morphing modes (more than bending) and local magnetic control remains challenging but is crucial for further on-demand applications. Here, we address the challenges by maximizing the unexplored potential of magnetothermal responsiveness and covalent adaptable networks (CANs) in liquid crystalline elastomers (LCEs). Various magneto-actuated contraction-derived motions that were hard to achieve previously (e.g., bidirectional shrinkage and dynamic 3D patterns) can be attained, reprogrammed, and assembled seamlessly to endow functional diversity and complexity. By integration of LCEs with different magneto-responsive threshold values, local and sequential magnetic control is readily realized. Many magnetic actuation portfolios are performed by rationally imputing “logic switch” sequences. Meanwhile, our systems exhibit additional favorable performances including stepwise magnetic controllability, multiresponsiveness, self-healing, and remolding ability.

Thermal reprogrammability is essential for new‐generation large dry soft actuators, but the realization sacrifices the favored actuation performance. The contradiction between thermal reprogrammability and stability hampers efforts to design high‐performance soft actuators to be robust and thermally adaptable. Now, a strategy has been developed that relies on repeatedly switching on/off thermal reprogrammability in liquid‐crystalline elastomer (LCE) actuators to resolve this problem. By post‐synthesis swelling, a latent siloxane exchange reaction can be induced in the common siloxane LCEs (switching on), enabling reprogramming into on‐demand 3D‐shaped actuators; by switching off the dynamic network by heating, actuation stability is guaranteed even at high temperature (180 °C). Using partially black‐ink‐patterned LCEs, selectively switching off reprogrammability allows integration of completely different actuation modes in one monolithic actuator for more delicate and elaborate tasks.

The search for ferroelectric materials that have a significant progress in applications, such as ferroelectric field-effect transducers, piezoelectric sensors, nonlinear optical devices, electrocaloric refrigeration, and so forth, remains a great challenge. Here, we report the discovery of two unique molecular ferroelectrics (TMP) 2 (SbX 5 )(SbX 3 ) (TMP = thiomorpholine = (CH 2 ) 4 NH 2 S + , X = Cl (1-Cl), Br (2-Br)), which are the first reported examples of halogenoantimonates(III) and halogenobismuthates(III) with R 2 (MX 5 )(MX 3 )-type zero-dimension (0D) configuration ascribing to the discrete SbX 5 and SbX 3 polyhedrons separated by the TMP cations. (TMP) 2 (SbX 5 )(SbX 3 ) also feature the highest phase transition temperature (T c , in which 362/442 K for 1-Cl and 385/477 K for 2-Br) and giant zero-field entropy change (131.68/109.16 J mol −1 K −1 for 1-Cl and 183.24/150.32 J mol −1 K −1 for 2-Br) in halogenoantimonates(III) and halogenobismuthates(III)-based molecular ferroelectrics. A low thr-coordinated SbX 3 component accelerates the crystallization of (TMP) 2 (SbX 5 )(SbX 3 ) in the noncentrosymmetric structure because it breaks the R 2 MX 5 -type construction. Thus, they exhibit significant room-temperature SHG signals (in which 4.2 × KDP for 1-Cl and 3.8 × KDP for 2-Br) and polarization-dependent SHG response. In addition, ultraviolet−visible absorption and photoluminescence spectra reveal that the band gap is successfully tuned from 3.366 to 2.600 eV for 1-Cl to 2-Br, while emission at 545 nm for 1-Cl is redshifted to 611 nm for 2-Br; both large Stokes shifts and broadband emission characterize the PL of 0D metal halide hybrids and are attributed to the strong coupling of the excitons to multiple phonons. This work will provide an avenue to explore the SHG responses and photoelectric characteristics of lowdimensional halogenoantimonates(III) and halogenobismuthates(III)-based molecular ferroelectrics.

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Lithium metal batteries (LMBs) have attracted widespread concern as the next‐generation energy storage devices with high energy density. At the surface of lithium metal anodes (LMAs) toward electrolytes, lithium plating always competes with interfacial reactions. This makes interfacial reactions light shadow right behind lithium plating, leading to performance degradation. Herein, lithium plating is spatially decoupled from interfacial reactions by constructing a 3D solid electrolyte interphase framework (3D‐SEIF) inside LMAs. Spontaneous while mild chemical reactions between lithium metal and lithium bisfluorosulfonimide/lithium nitrate form the robust 3D‐SEIF, mainly consisting of LiF, Li3N, and LiNxOy. The built‐in 3D‐SEIF avoids electrolyte contact but enables the diffusion and reduction of Li+ ions in the bulk phase, thus isolating the plating sites and electrolyte contact interface. The 3D‐SEIF facilitates large granular plating and the generation of thin, inorganic‐rich SEI. When assembled with high‐loading LiNi0.6Co0.2Mn0.2O2 cathode (3 mAh cm−2), the cells present capacity retention of 92.0% after 130 cycles with barren electrolyte (≈30 µL) at 0.5 C. The conception of 3D inner interphase allows breaking the coupling of interfacial reactions with electrochemical reactions, which is taken for granted in electrochemical consortium. It also desires to inspire new thoughts to develop scalable solutions for the early industrialization of LMBs.