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Page 2 of 8                            Xiao et al. Soft Sci. 2025, 5, 40  https://dx.doi.org/10.20517/ss.2025.51

               INTRODUCTION
               With the rapid advance of flexible electronics, wearable sensors that form high-performance interfaces with
               human skin are gradually replacing conventional rigid devices and have become indispensable in health
               monitoring , active rehabilitation , and intelligent human-machine interaction (HMI) . Among the
                         [1-3]
                                             [4,5]
                                                                                             [6-8]
               various soft electronic materials under development, hydrogels stand out because their physicochemical
               characteristics closely resemble those of human skin [9-14] . When used as epidermal electrodes, hydrogel
               devices can record diverse biosignals - such as electroencephalograms (EEG) and surface electromyograms
               (sEMG) - and supply them as high-value inputs to HMI systems [15,16] .


               High-performance HMI platforms rely on electrophysiological signals with a high signal-to-noise ratio
                    [17]
               (SNR) . Achieving such quality depends on a low-impedance hydrogel-skin interface that minimizes signal
               attenuation and external interference . Excellent electrical conductivity of hydrogel electrodes is demanded
                                              [18]
               to support efficient signal transmission. Simultaneously, sufficient mechanical flexibility is required to
               conform intimately to the microtopography of the skin . Moreover, strong adhesive properties are
                                                                 [19]
               necessary to prevent electrode displacement during movement and enable stable and continuous biosignal
               monitoring [Figure 1A] . However, conventional hydrogels often suffer from poor conductivity, weak
                                    [20]
               adhesion, and mechanical mismatch with skin, compromising signal quality . Therefore, next-generation
                                                                                [19]
               hydrogel electrodes must be engineered with conductive additives, ions, adhesion enhancers, and
               multidimensional structural optimizations to ensure long-term, stable collection of high-quality
               physiological data for advanced HMI applications.

               PERFORMANCE OPTIMIZATION STRATEGIES AND INTERFACE ENGINEERING OF
               HYDROGEL ELECTRODES
               The three-dimensional network of hydrogels offers intrinsic porosity for incorporating functional fillers,
               enabling optimization of conductivity, adhesion, and mechanical compliance to enhance skin-electrode
               interfaces [21,22] . Common strategies include adding fillers such as tannic acid (TA) and MXene, which
                                                                                                       [23]
               improve both conductivity and adhesion, ensuring a low-impedance and stable skin-electrode interface .
               For example, Wan et al. integrated MXene nanosheets into a self-healing hydrogel made of TA-
               phenylboronic acid-grafted hyaluronic acid (HA-PBA) [Figure 1B] , resulting in a stable skin interface that
                                                                       [24]
               supports multimodal biosignal acquisition and additional functions such as ultraviolet (UV) protection and
               photothermal therapy via MXene’s photothermal conversion ability. Furthermore, Wu et al. introduced TA
               into a polyacrylamide (PAM) hydrogel and immersed it in sodium chloride (NaCl) solution, enhancing
               ionic conductivity and enabling high-performance signal acquisition from hairy skin surfaces [Figure 1C] .
                                                                                                       [17]
               In addition to TA, polydopamine (PDA) is also a commonly used functional filler to improve the adhesive
               and mechanical properties of hydrogel electrodes. For example, Han et al. added PDA nanoparticles to a
               polyvinyl alcohol (PVA)/polyvinylpyrrolidone (PVP) hydrogel [Figure 1D], improving adhesion and
               enabling stable attachment to various surfaces, including skin, metal, and glass [Figure 1E] . This electrode
                                                                                           [19]
               showed low interface impedance, ensuring stable EEG signal acquisition [Figure 1F]. PDA and TA enhance
               adhesion through hydrogen bonds and π-π interactions with skin proteins, improving interfacial stability
               during movement [17,19] . Liquid metal is another filler that boosts conductivity and flexibility, making
               hydrogels suitable for dynamic, stretchable applications . Hu et al. incorporated liquid metal into a dual-
                                                               [1]
               network hydrogel of PAM and gelatin, achieving high conductivity and intelligent adhesiveness [Figure
                  [25]
               1G] , resulting in superior sEMG signal acquisition compared to commercial electrodes. This hydrogel
               maintained stable signal acquisition for up to 48 h, showing promise for wearable bioelectronics
               [Figure 1H].
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