In this paper, a titanium pyrophosphate (TiP2O7) anode with oxygen vacancies is prepared by a simple one-pot solid method, exhibiting great performance. Herein, we study on the physical and chemical changes of TiP2O7-y with oxygen defect, and compare it with pure TiP2O7 through scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and so on. It is found that the introduction of oxygen vacancies leads an improved electronic conductivity compared to the pure TiP2O7 sample. Intriguingly, the TiP2O7-y with oxygen defect displays an enhanced electrochemical performance in aqueous lithium ion batteries (ALIBs), with a larger capacity of TiP2O7-y (57 mAh g−1) as compared to pure TiP2O7 (17 mAh g−1) at 0.2 A g−1. After carbon-coating treatment, the C–TiP2O7-y anode demonstrates outstanding capacity and cycling performance with a capacity retention of 89% after 500 cycles at 0.5 A g−1. More importantly, the full ALIBs coupled with LiMn2O4 cathode maintains 85% capacity after 800 cycles at 0.1 A g−1. This study underscores the potential importance of incorporating oxygen vacancies into metal oxides as an alternative to modify the electrode materials in energy storage field.