TEMPO-oxidized nanofibrillated cellulose (ONFC) with charged carboxyl groups is introduced for the efficient exfoliation of two-dimensional (2D) MoS2 /graphene composites. As an effective dispersant agent, ONFC can be easily absorbed between the adjacent layers, so as to prevent the accumulation of the exfoliated nanosheets. With the assistance of charged ONFC, the exfoliated MoS2 /graphene is gradually increased in the aqueous dispersions with the elongated sonication time. After dewatering, self-standing MoS2 /Graphene/ONFC/CNTs composite films are rationally constructed using ONFC as flexible fibrous skeleton, and CNTs/graphene as 1D/2D interpenetrating electrical networks. Ultrathin MoS2 nanosheets anchored on the 1D/2D heterogeneous networks is directly acted as an ideal paper-anode for lithium-ion batteries (LIBs) without using traditional metallic current collector. The self-standing flexible electrode materials based on natural cellulose will promote the future green electronics with high flexibility, miniaturization, and increased portability.