Spiropyran‐based materials (SPBMs) can give responses to the stimulations induced by the light, heat, force, or pH, which have been used as triggers for many smart materials. Here, a cross‐linkable SPBM containing mesogenic‐units is synthesized, which is pale‐colored, non‐photoluminescent and non‐mesogenic at a spiro form, but dark‐colored, photoluminescent, and mesogenic at a merocyanine form. Moreover, the dynamic interconversion behavior of the form in the different chemical environments are distinct. Liquid crystalline polymers (LCPs) containing the SPBMs cross‐linked via visible light, own a photoswitchable glass transition temperature (Tg) and retain the switchable property; however, the SPBMs cross‐linked via UV light will be locked at the MC state, because the molecular movement was frozen at the room temperature lower than the given Tg of the LCP. Thus, programmable chromism and photoluminescence based on the tunable Tg can be endowed to the functional materials prepared from the SPBMs.

The ability of some animals to rapidly change their colors can greatly improve their chances of escaping predators or hunting prey. A classic example is cephalopods, which can rapidly shift through a wide range of colors. This ability is based on the synergetic effect of the change of pigmentary and structural colors exhibited by their own two categories of color‐changing cells: supernatant chromatophores offer various pigmentary colors and lower iridophores or leucophores reflect the different structural colors by adjusting their periodicities. Here, a mechanochromic liquid crystalline elastomer with force‐induced synergetic pigmentary and structural color change, whose mechanosensitivity is enhanced by the stress‐concentration induced by the doped nanoparticle, is presented. The materials have a large color‐changing gamut and high mechanochromic sensitivity, which exhibit great potential in the field of mechanical detectors, sensors, and anti‐counterfeiting materials.

Solid polymer electrolytes (SPEs) have emerged as one of the most promising candidates for building solid‐state lithium batteries due to their excellent flexibility, scalability, and interfacial compatibility with electrodes. However, the low ionic conductivity and poor cyclic stability of SPEs do not meet the requirements for practical applications of lithium batteries. Here, a novel polymer dispersed ionic liquid‐based solid polymer electrolyte (PDIL‐SPE) is fabricated using the in situ polymerization‐induced phase separation (PIPS) method. The as‐prepared PDIL‐SPE possesses both outstanding ionic conductivity (0.74 mS cm−1 at 25°C) and a wide electrochemical window (up to 4.86 V), and the formed unique three‐dimensional (3D) co‐continuous structure of polymer matrix and ionic liquid in PDIL‐SPE can promote the transport of lithium ions. Also, the 3D co‐continuous structure of PDIL‐SPE effectively accommodates the severe volume expansion for prolonged lithium plating and stripping processes over 1000 h at 0.5 mA cm−2 under 25°C. Moreover, the LiFePO4//Li coin cell can work stably over 150 cycles at a 1 C rate under room temperature with a capacity retention of 90.6% from 111.1 to 100.7 mAh g−1. The PDIL‐SPE composite is a promising material system for enabling the ultrastable operation of solid‐state lithium‐metal batteries.

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