Rational design and construction of advanced hybrid electrodes would contribute to enormous development of rechargeable batteries. Herein, hierarchical accordion-like TiO2/Ti3C2 nanohybrid is purposefully synthesized by using Ti3C2 as single precursor through a scalable hydration process, and further evaluated as promising anode material both for Li-ion batteries (LIBs) and Na-ion batteries (SIBs). Physicochemical characterizations demonstrate that the unique hierarchical nanohybrid possesses a layered architecture, where the in-situ formed nanoscaled TiO2 is decorated uniformly on the Ti3C2 surface. Benefiting from synergetic contributions from interlayer-expanded architecture, high-capacity nano-TiO2 and excellent electrical conductivity of the Ti3C2, the resulted TiO2/Ti3C2 anode exhibits large reversible capacities of ∼267 and ∼101 mAh g−1 for LIBs and SIBs, respectively, at a current density of 200 mA g−1. Moreover, no any capacity decay over consecutive 500, and even 2000 cycles at high rates further confirms its outstanding electrochemcial stability for practical applications. More appealingly, all the results highlight that the cost-efficiency TiO2/Ti3C2 hybrid architecture would be a promising anode candidate for advanced next-generation LIBs and SIBs.