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A substantial increase in charging capacity over long cycle periods was made possible by the formation of a flexible weblike network via the combination of Al₂O₃ atomic layer deposition (ALD) and the electrolyte additive vinylene carbonate (VC). Transmission electron microscopy shows that a weblike network forms after cycling when ALD and VC were used in combination that dramatically increases the cycle stability for the Si composite anode. The ALD–VC combination also showed reduced reactions with the lithium salt, forming a more stable solid electrolyte interface (SEI) absent of fluorinated silicon species, as evidenced by X-ray photoelectron spectroscopy. Although the bare Si composite anode showed only an improvement from a 56% to a 45% loss after 50 cycles, when VC was introduced, the ALD-coated Si anode showed an improvement from a 73% to a 11% capacity loss. Furthermore, the anode with …