The synthesis and characterization of layered double hydroxide (LDH) and intercalated polyoxometalate are presented. We have reported the growth of polyoxometalate on (Ni, Mg) layered double hydroxide for degradation procion red (PR). The degradation parameters and organic dye removal efficiency of Zn/Mg-LDH and both composite LDH-polyoxometalate have been determined by considering factors such as pH of dye solution, catalyst dosage, and time as variables of degradation. X-Ray, FTIR, and SEM spectroscopy confirmed the layered double hydroxide structure. XRD and FTIR analysis confirmed the single-phase of the as-made and polyoxometalate intercalated LDH. SEM images show the formation of aggregates of small various sizes. The catalytic activity of the material was evaluated in the degradation of PR as a model pollutant. The result showed that MgAl-SiW12O40 has a good degradation capacity for PR as compared to MgAl-PW12O40, ZnAl-SiW12O40, and ZnAl-PW12O40. The result shows that the LDH composite presents stability and has good photocatalytic activities toward the reduction of procion red. The materials utilized for the fifth regeneration are indicated by the FTIR results, which verified the LDH composite structure. The PR’s photodegradation process for immaculate ZnAl-LDH, MgAl-LDH, ZnAl-[PW12O40], ZnAl-[SiW12O40], MgAl-[PW12O40], MgAl-[SiW12O40] were 68%, 70%, 56%, 79%, 74%, and 80%. The LDH-polyoxometalate composite material’s capacity to successfully photodegrade, as measured by the percentage of degradation, revealed an increase in photodegradation catalysis and the ability of LDH to regenerate.