The performance of poly(N-vinylcarbazole) (PVK) for use in rechargeable lithium batteries was investigated. The positive-electrode (cathode) using PVK as an active material exhibited a discharge capacity of more than 120mAhg−1 (PVK) with a mean potential of 3.7V vs. Li+/Li. The PVK-electrode showed a stable cycle-life performance. In addition, the application of this polymer as a redox active binder material was also examined using a composite electrode with lithium iron phosphate (LiFePO4). The LiFePO4–PVK composite electrode showed a higher total discharge capacity than the conventional LiFePO4–PVDF electrode.