Abstract Organic carbonyl electrode materials are widely employed for alkali metal‐ion secondary batteries in terms of their sustainability, structure designability and abundant resources. As a typical redox‐active organic electrode materials, pyrene‐4, 5, 9, 10‐tetraone (PT) shows high theoretical capacity due to the rich carbonyl active sites. But its electrochemical behavior in secondary batteries still needs further exploration. Herein, PT‐based linear polymers (PPTS) is synthesized with thioether bond as bridging group and then employed as an anode material for lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs). As expected, PPTS shows improved conductivity and insolubility in the non‐aqueous electrolyte. When used as an anode material for LIBs, PPTS delivers a high reversible specific capacity of 697.1 mAh g −1 at 0.1 A g −1 and good rate performance (335.4 mAh g −1 at 1 A g −1 ). Moreover, a reversible specific capacity of 205.2 mAh g −1 at 0.05 A g −1 could be obtained as an anode material for SIBs.