Redeeming water from heavy metal contaminants has arisen global concerns due to water shortage and lax control on the discharge of heavy metal pollutants. Capacitive deionization (CDI) has emerged as a robust, energy-/cost-efficient technique for water treatment. Herein, we reported the simple N,S-codoped carbon materials (NS-C) from PVC plastic wastes as CDI electrode materials for the efficient removal of heavy metal ions (HMI). The NS-C exhibited large specific surface area (~1230 m2 g-1) and contained heavy heteroatom doping (~4.55 at.% N and ~13.30 at.% S). CDI electrode fabricated using NS-C showed very high removal efficiency (94-99%), high capacity (36-62 mg g-1), and good regeneration capability for the adsorption of various kinds of low-concentration heavy metals ions (including Fe2+, Co2+, Ni2+, Cu2+, Pb2+, and Cd2+). Moreover, PVC plastic wastes that are heavily accumulated in the environment and extremely hard to be decomposed and recycled were applied as carbon source in this study for the fabrication of NS-C, which further rendered the importance of our study to practically treating hazardous wastes (HMI pollutions) with wastes (PVC plastic wastes) in clean and efficient way.