Reduction of nitroarenes is a highly versatile conversion that still remains a challenge in controlling functionality and adjustments on MOFs. On the other hand, offers an attractive opportunity to expand their applications in designing the next generation of catalysts with improved performance. Herein, a novel MOF consisting of supported triazine-aminopyridine (MIL-101(Cr)-NH-TA-AP) has been synthesized using triazine and 2-aminopyridine ligands. Subsequently, to impart catalytic sites, the prepared nanocomposites were modified using Ni NPs (MIL-101(Cr)-NH-TA-AP/Ni). Then, an efficient method for the synthesis of new thiourea derivatives was developed by the reaction of nitrobenzene derivatives and phenyl isocyanate using of MIL-101(Cr)-NH-TA-AP/Ni/sodium borohydride in water. Based on the results, the active surface area of the synthesized nanocatalyst is large, which highlights its unique synergistic effect between post-synthetic modified MOF and Ni NPs.