We present an experimental platform of operando nanoindentation that probes the dynamic mechanical behaviors of electrodes during real-time electrochemical reactions. The setup consists of a nanoindenter, an electrochemical station, and a custom fluid cell integrated into an inert environment. We evaluate the influence of the argon atmosphere, electrolyte solution, structural degradation and volumetric change of electrodes upon Li reactions, as well as the surface layer and substrate effects by control experiments. Results inform on the system limitations and capabilities, and provide guidelines on the best experimental practices. Furthermore, we present a thorough investigation of the elastic-viscoplastic properties of amorphous Si electrodes, during cell operation at different C-rates and at open circuit. Pure Li metal is characterized separately. We measure the continuous evolution of the elastic modulus, hardness, and creep stress exponent of lithiated Si and compare the results with prior reports. operando indentation will provide a reliable platform to understand the fundamental coupling between mechanics and electrochemistry in energy materials. photovoltaics, 7 and hydrogen storage. 8 The electrochemical reactions between the host material and guest species induce deformation, stress, fracture, and fatigue which cause ohmic and thermal resistance increase, and performance degradation. Likewise, mechanical stresses regulate mass transport, charge transfer, interfacial reactions, and consequently the potential and capacity of electrochemical systems. 9 In batteries, mechanical degradation compromises the performance of current technologies [10][11][12] and limits the implementation of high-capacity electrodes.13,14 Mechanics of both anode and cathode materials, such as diffusion-induced stresses, large deformation, plasticity, and fracture, have been extensively studied in recent years. [15][16][17][18][19][20] Nevertheless, the intimate coupling between mechanics and electrochemistry is far from complete understanding despite a considerable volume of existing studies. One major deficiency is the lack of reliable experimental tools to characterize the mechanical behaviors of electrodes under real electrochemical conditions. The operation of batteries is extremely sensitive to the work environment -a trace of oxygen and moisture can cause numerous side reactions. In contrast, most mechanical test equipment is open system with limited capability of environment control. As such, the mechanics and electrochemistry of batteries are often characterized separately. Recent studies propose that the mechanical response of materials at the chemical equilibrium states may differ from that under concurrent mechanical and chemical loads. 21,22 There is an urgent need for an experimental platform to probe the chemomechanical behaviors of electrodes in the course of electrochemical reactions. Current experimental tools have been able to provide valuable insight. Due to the generally small characteristic size and heterogen...