Graphene nanoscrolls encapsulated TiO2 (B) nanowires have been fabricated through a self-scrolling and template-free process for the first time. Transmission electron microscope images reveal that graphene tightly encompassed TiO2 (B) nanowires to construct nanoscrolled architectures. Cyclic voltammetry demonstrates that pseudocapacitive behavior dominates fast lithium storage rather than diffusion-controlled insertion in the hybrids. Galvanostatic cycling tests show that the reversible specific capacity of the hybrids remains 153 mAh g−1 after 300 cycles at 10 C with capacity retention of 94%. The excellent lithium storage performance can be attributed to the unique nanoscrolled structure, which provides abundant channels for lithium ions transport, as well as accommodates volume variation during fast lithiation and delithiation.