The extensive utilization of chromium in electroplating, leather tanning, dyeing, and other industries has resulted in significant environmental pollution. Therefore, there is a pressing need for highly efficient materials to tackle the pollution caused by Cr(VI). Throughout the study, a variety of layered double hydroxides (LDHs) were synthesized, and the NiCr-LDH showed remarkable removal properties for the heavy metal chromium. The NiCr-LDH exhibits rapid equilibrium within 60 min and possesses a maximum capacity of 218 mg/g. Notably, when exposed to visible light, the ability of NiCr-LDH to remove toxic Cr(VI) anions is significantly improved, and it is capable of treating actual electroplating wastewater to remove the Cr concentration to well below 0.5 mg/L. In-depth analysis revealed compelling evidence that the highly toxic Cr(VI) anions transformed into harmless Cr(III) anions, resulting in an improved removal efficiency.