The synthesis of layered freestanding papers composed of acid-functionalized, few-layer molybdenum disulfide (MoS2) and reduced graphene oxide (rGO) flakes for use as a binder-free conducting electrode in NIB applications are described. The mechanical and electrochemical performance of the layered freestanding papers is also described. Synthesis was achieved through vacuum filtration of highly homogenous dispersions comprising varying weight percentages of exfoliated MoS2 flakes in graphene oxide in DI water, followed by thermal reduction. The electrochemical behavior of the composite paper was evaluated as a counter electrode against pure Na foil in a half-cell configuration. In addition, the uniaxial tensile testing of the composite papers demonstrated their exceptionally high fracture strength.