A new facile route to fabricate N-doped graphene-SnO2 sandwich papers is developed. The 7,7,8,8-tetracyanoquinodimethane anion (TCNQ-) plays a key role for the formation of such structures as it acts as both the nitrogen source and complexing agent. If used in lithium-ion batteries (LIBs), the material exhibits a large capacity, high rate capability, and excellent cycling stability. The superior electrochemical performance of this novel material is the result from its unique features: excellent electronic conductivity related to the sandwich structure, short transportation length for both lithium ions and electrons, and elastomeric space to accommodate volume changes upon Li insertion/extraction.