Heterometallic Gd−Pt complexes ([Gd2Pt3(H2O)2(SAc)12] (SAc=thioacetate), [Y1.4Gd0.6Pt3(H2O)2(SAc)12], and [Gd2Pt3(H2O)6(SAc)12]⋅7 H2O have been synthesized. The crystal structures and DFT calculations indicated a Gd−Pt heretometallic bond. Single-crystal ESR spectra determined the direction of magnetic anisotropy as direction of the Gd−Pt bond. In other words, the Gd−Pt bond dictates the direction of magnetic anisotropy. The heterometallic Gd−Pt bond lowers the symmetry of the Gd ion, splitting the Kramers doublet in a dc field. Thus, we observed clear field-induced slow magnetic relaxation of [Y1.4Gd0.6Pt3(H2O)2(SAc)12] up to 36 K. The relaxation process was determined to be a direct process.