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This tandem process is efficiently accomplished in the presence of a cubane\u2010type Mo<jats:sub>3<\/jats:sub>PtS<jats:sub>4<\/jats:sub> catalyst. For the preparation of the novel [Mo<jats:sub>3<\/jats:sub>Pt(PPh<jats:sub>3<\/jats:sub>)S<jats:sub>4<\/jats:sub>Cl<jats:sub>3<\/jats:sub>(dmen)<jats:sub>3<\/jats:sub>]<jats:sup>+<\/jats:sup> (<jats:bold>3<\/jats:bold><jats:sup>+<\/jats:sup>) (dmen: <jats:italic>N<\/jats:italic>,<jats:italic>N\u2032<\/jats:italic>\u2010dimethylethylenediamine) compound we have followed a [3+1] building block strategy starting from the trinuclear [Mo<jats:sub>3<\/jats:sub>S<jats:sub>4<\/jats:sub>Cl<jats:sub>3<\/jats:sub>(dmen)<jats:sub>3<\/jats:sub>]<jats:sup>+<\/jats:sup> (<jats:bold>1<\/jats:bold><jats:sup>+<\/jats:sup>) and Pt(PPh<jats:sub>3<\/jats:sub>)<jats:sub>4<\/jats:sub> (<jats:bold>2<\/jats:bold>) complexes. The heterobimetallic <jats:bold>3<\/jats:bold><jats:sup>+<\/jats:sup> cation preserves the main structural features of its <jats:bold>1<\/jats:bold><jats:sup>+<\/jats:sup> cluster precursor. Interestingly, this catalytic protocol operates at room temperature with high chemoselectivity when the <jats:bold>3<\/jats:bold><jats:sup>+<\/jats:sup> catalyst co\u2010exists with its trinuclear <jats:bold>1<\/jats:bold><jats:sup>+<\/jats:sup> precursor. N\u2010heterocyclic arenes, double bonds, ketones, cyanides and ester functional groups are well retained after <jats:italic>N<\/jats:italic>\u2010methylation of the corresponding functionalized nitroarenes. 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