Electrode cracking is a serious problem that hinders the application of many next-generation high-capacity anode materials for lithium-ion batteries. Even though nano-sizing the material can reduce fracturing of individual particles, capacity fading is still observed due to large volume change and loss of contact in the electrode during lithium insertion and extraction. In this study, we design a crack-resistant high-modulus polyimide coating with high compressive strength which can hold multiple particles together during charge and discharge to maintain contact. The effectiveness of the coating is demonstrated on tin dioxide, a high-capacity large-volume-change material that undergoes both alloy and conversion reactions. The polyimide coating improves capacity retention of SnO2 from 80% to 100% after 80 cycles at 250 mA g−1. Stable capacity of 585 mAh g−1 can be obtained even at 500 mA g−1 after 300 cycles. Scanning electron microscopy and in-situ dilatometry confirm that electrode cracking is suppressed and thickness change is reduced with the coating. In addition, the chemically-stable polyimide film can separate the surface from direct contact with electrolyte, improving coulombic efficiency to ∼100%. We expect the novel strategy of suppressing electrode degradation with a crack-resistant coating can also be used for other alloy and conversion-based anodes.