Exploring materials with high electrochemical activity is of keen interest for electrochemistry-controlled optical and energy storage devices. However, it remains a great challenge for transition metal oxides to meet this feature due to their low electron conductivity and insufficient reaction sites. Here, we propose a type of transition metal phosphate (NiHPO4·3H2O, NHP) by a facile and scalable electrodeposition method, which can achieve the capability of efficient ion accommodation and injection/extraction for electrochromic energy storage applications. Specifically, the NHP film with an ultra-high transmittance (approach to 100%) achieves a large optical modulation (90.8% at 500 nm), high coloration efficiency (75.4 cm2 C−1 at 500 nm), and a high specific capacity of 47.8 mAh g−1 at 0.4 A g−1. Furthermore, the transformation mechanism of NHP upon electrochemical reaction is systematically elucidated using in situ and ex situ techniques. Ultimately, a large-area electrochromic smart window with 100 cm2 is constructed based on the NHP electrode, displaying superior electrochromic energy storage performance in regulating natural light and storing electrical charges. Our findings may open up new strategies for developing advanced electrochromic energy storage materials and smart windows.

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Polymer‐dispersed liquid crystal (PDLC) devices are truly promising optical modulators for information display, smart window as well as intelligent photoelectronic applications due to their fast switching, large optical modulation as well as cost‐effectiveness. However, realizing highly soft PDLC devices with sensing function remains a grand challenge because of the intrinsic brittleness of traditional transparent conductive electrodes. Here, inspired by spiderweb configuration, a novel type of silver nanowires (AgNWs) micromesh‐based stretchable transparent conductive electrodes (STCEs) is developed to support the realization of soft PDLC device. Benefiting from the embedding design of AgNWs micromesh in polydimethylsiloxane (PDMS), the STCEs can maintain excellent electrical conductivity and transparency even in various extreme conditions such as bending, folding, twisting, stretching as well as multiple chemical corrosion. Further, STCEs with the embedded AgNWs micromesh endow the assembled PDLC device with excellent photoelectrical properties including rapid switching speed (<1 s), large optical modulation (69% at 600 nm), as well as robust mechanical stability (bending over 1000 cycles and stretching to 40%). Moreover, the device displays the pressure sensing function with high sensitivity in response to pressure stimulus. It is conceivable that AgNWs micromesh transparent electrodes will shape the next generation of related soft smart electronics.

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