Utilizing graphene-based hybrid papers or films as multifunctional electrodes has become the focus of clean energy devices due to the beneficial combination of their excellent electrical properties and multiple functions. However, limited attention has been paid to such hybrid papers with both outstanding mechanical and electrochemical properties. Recently, we fabricate rationally designed TiO2-B nanofibrils reinforced graphene paper, which can achieve high mechanical strength (88.5 MPa) without sacrificing their electrochemical properties. They further deliver capacities of 231 mAh g−1 (408.9 mAh cm−3) for Li-ion electrode and 201 mAh g−1 (355.8 mAh cm−3) for Na-ion electrode respectively at the same current density of 33.5 mA g−1. The outstanding mechanical stability of as-prepared hybrid electrode is demonstrated with a prototype of a bendable Li-ion capacitor. Besides, the as-prepared electrodes also reveal great potential to serve as light weight and ultrathin electromagnetic interference shielding materials. Single layer of hybrid paper exhibits a shielding effectiveness of over 10 dB (corresponding ∼90% shielding). These results prove that TiO2-B nanofibrils reinforced graphene paper can serve as a multifunctional flexible electrode for diverse applications. Moreover, this work also demonstrates a novel strategy on how to enhance mechanical properties for those flexible electrodes.