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Hollow structures of transition metal sulfides, could be promising for energy devices such as hybrid supercapacitors, lithium ion batteries (LIBs) and sodium ion batteries (SIBs). Specially, mixed transition metal sulfides, benefiting from synergetic effects of the multiple metal species, have shown significant advance in the electrochemical performances of LIBs. Whereas, there is no report on exploring them as the electrode materials for sodium ion batteries (SIBs). Herein, we reported the successful fabrication of Zn0.33Co0.67S hollow microspheres with well‐defined voids via a novel sulfidation into ZnCo2‐glycolate solid microspheres and employed them as the electrodes in rechargeable secondary batteries like LIBs and SIBs. Specifically, in LIB testing, the Zn0.33Co0.67S hollow microsphere electrodes delivered a reversible capacity of 540 mA h g–1 at the current density of 500 mA g–1 over 200 cycles. Interestingly, as the pioneering anode among mixed transition sulfides in SIBs, Zn0.33Co0.67S hollow microsphere electrodes still stored Na+ as high as 420 mA h g–1 at 500 mA g–1 over 50 sodiation/desodiation repeating cycles. [ABSTRACT FROM AUTHOR]