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The application of oxygen-deficient perovskites (ODPs) has attracted interest as anode materials for lithium-ion batteries for their unique properties. One such material, CaSrFe0.75Co0.75Mn0.5O6-δ, has been studied extensively. The structure of CaSrFe0.75Co0.75Mn0.5O6-δ was investigated using various techniques, including Rietveld refinements with X-ray diffraction and neutron diffraction. Additionally, iodometric titration and X-ray photoelectron spectroscopy were employed to study the oxygen-deficiency amount and the transition metal’s oxidation states in the material. As an anode material, CaSrFe0.75Co0.75Mn0.5O6-δ exhibits promising performance. It delivers 393 mAhg−1 of discharge capacity at a current density of 25 mAg−1 after 100 cycles. Notably, this capacity surpasses both the theoretical graphite anode capacity (372 mAhg−1) and that of the calcium analog reported previously. Furthermore, the electrochemical performance of CaSrFe0.75Co0.75Mn0.5O6-δ remains highly reversible across various current densities ranging from 25 to 500 mAg−1. This suggests the material’s excellent stability and reversibility during charge–discharge cycles, showing its probable application as an anode for lithium-ion batteries. The mechanism of lithium intercalation and deintercalation within CaSrFe0.75Co0.75Mn0.5O6-δ has also been discussed. Understanding this mechanism is crucial for optimizing the battery’s performance and ensuring long-term stability. Overall, this study highlights the significant potential of oxygen-deficient perovskites, particularly CaSrFe0.75Co0.75Mn0.5O6-δ, for applications as an anode material for lithium-ion batteries, offering enhanced capacity and stability compared with traditional graphite-based anodes.