In this work, cellulose acetate polymer (CA) sheet and 2% ZnAl grafted on activated carbon grown in the form of layered double hydroxide (ZnAl/C-LDH) incorporated into CA polymer (CA-ZA2) 5 wt% (CA-ZA5) and 10 wt% of ZnAl/C-LDH (CA-ZA10) sheets were synthesized by simple casting method. All the stated sheets were fabricated with zero-valent Ni nanoparticles by adsorption of Ni ions followed by subsequent reduction with NaBH and named as CA@Ni, CA-ZA2@Ni, CA-ZA5@Ni, and CA-ZA10@Ni NPs. The synthesized Ni NPs were investigated through FESEM, FTIR, XRD and EDS techniques. These supported and stabilized Ni NPs were largely used for the reduction of 4-nitrophenol (PNP), and 2-nitrophenol (ONP) in the presence of NaBH which act as a reducing agent. Similarly, the catalytic efficiency was also assessed against the removal of dyes. The linear relationship and K were obtained from pseudo-first-order kinetics. The rate constant K of CA@Ni NPs for the reduction of PNP is 1.5 × 10 and CA-ZA2@Ni (K = 2.6 × 10), CA-ZA5@Ni (K = 3.2 × 10), and CA-ZA10@Ni is 5.7 × 10 min. The highest rate constant for PNP reduction was observed with CA-ZA10@Ni NPs. The rate of CR removal with ZA10@Ni NPs is 2.05 × 10 while the adjacent R is 0.9013. Similarly, the rate constant and adjacent R values were calculated for the degradation of other dyes and nitrophenols.