The novel sulfomethylated lignin-grafted-polyacrylic acid (SL-g-PAA) hydrogel was fabricated in this work via a facile and green synthetic strategy for the efficient removal of heavy metal ions from wastewater, and then successively reused for chemiluminescence (CL). The sulfomethylation of lignin was first performed to improve its water solubility and introduce numerous active sites for adsorption of heavy metal ions. The as-synthesized SL-g-PAA hydrogel with high content of lignin exhibited the highly efficient and rapid removal of various metal ions from simulated wastewater. More importantly, the spent hydrogel (M2+@SL-g-PAA) after adsorption was reused for the first time to develop a new CL system by an ingenious strategy, in which these metal ions adsorbed on M2+@SL-g-PAA act as heterogeneous catalytic sites to catalyze the CL reaction between N-(4-aminobutyl)-N-ethylisoluminol (ABEI) and H2O2. The resultant CL system displayed high CL intensity and long duration time, which could be observed by naked eye in the dark and lasted for > 24 h. The combination of facile fabrication process, renewable raw materials, and ingenious strategy for successive application in adsorption and CL endows this lignin-based composite hydrogel with a great potential for application in wastewater treatment, biological imaging and cold light sources. Display omitted •A lignin-based hydrogel was fabricated by a facile and green synthetic strategy.•SL-g-PAA exhibited efficient and rapid removal of heavy metal ions from wastewater.•Spent hydrogel after adsorption was reused for the first time to develop CL system.•A highly intensive and long-lasting CL system was obtained by an ingenious design.•A new strategy for successive application of lignin-based hydrogels was presented.