Reversible Li-ion intercalation into composite Liion battery (LIB) electrodes is often accompanied by significant dimensional electrode changes (deformation) resulting in significant deterioration of the cycling performance.V iscoelastic properties of polymeric binders affected by intercalation-induced deformation of composite LIB electrodes have never been probed in situ on operating electrochemical cells. Here,w ei ntroduce an ewly developed noninvasive method, namely electrochemical quartz-crystal microbalance with dissipation monitoring (EQCM-D), for in situ monitoring of elastic properties of polymeric binders during charging of LIB electrodes.A ss uch,w ef ind EQCM-D as au niquely suitable tool to trackthe binders structural rigidity/softness in composite Li insertion electrodes in real-time by the characteristic increase/decrease of the dissipation factor during the chargingdischarging process.T he binders partially swollen in aprotic solutions demonstrate intermediate viscoelastic charge-ratedependent behavior,r evealing rigid/soft behavior at high/low charging rates,r espectively.T he method can be adjusted for continuous monitoring of elastic properties of the polymeric binders over the entire LIB electrodes cycling life.Lithium-ion batteries (LIB) offer av ery broad spectrum of applications,from portable devices to larger scale all-electric vehicles. [1] Forl arge-scale applications,p orous composite LIBs electrodes are usually used, containing at least three components:e lectrode particles (e.g.,L iFePO 4 ), ab inder (commonly,p olyvinylidene fluoride,P VdF,a nd sodium carboxymethylcellulose,NaCMC), [2] and conductive additives such as carbon black, graphene,o rc arbon nanotubes.T he processes of ions extraction/insertion occurring in LIBs electrodes during their charge/discharge result in periodic potential-dependent changes of the electrodes volume (i.e., their deformation), bringing about av ariety of undesirable mechanical effects,s uch as high-enough stresses,f atigue, fracture,a nd delamination from current collector. [3] Current techniques for in situ monitoring of electrodes strains include atomic force microscopy (AFM) [4] and electrochemical dilatometry. [5] Ac ommon drawback of these techniques is that they do not provide direct information on the potentialinduced changes of the electrode porosity,w hich is an important factor of stress relaxation in LIB electrodes.It has been recently shown that electrochemical quartzcrystal microbalance (EQCM) has at remendous benefit of direct in situ gravimetric probing of ionic fluxes into composite nanoporous carbon electrodes during charging and discharging. [6] Later we have developed as elf-consistent in situ methodology for tracking dimensional changes of this electrode based on EQCM with dissipation monitoring (EQCM-D) and we demonstrated this methods potential for two systems:L iFePO 4 olivine as at ypical composite intercalation-type LIB cathodes material [7] and Ti 3 C 2 M x MXene as acomposite material with properties intermediate between b...