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The crystal structure of compound <jats:bold>4<\/jats:bold> consists of discrete heterotrimetallic complex cations, [Cu<jats:sup>II<\/jats:sup>(valpn)La<jats:sup>III<\/jats:sup>(OH<jats:sub>2<\/jats:sub>)<jats:sub>3<\/jats:sub>(O<jats:sub>2<\/jats:sub>NO)(\u03bc\u2010NC)Fe<jats:sup>III<\/jats:sup>(phen)(CN)<jats:sub>3<\/jats:sub>]<jats:sup>+<\/jats:sup>, nitrate counterions, and non\u2010coordinate water and acetonitrile molecules. The heteroleptic {Fe<jats:sup>III<\/jats:sup>(bipy)(CN)<jats:sub>4<\/jats:sub>} moiety in <jats:bold>5<\/jats:bold>\u2013<jats:bold>7<\/jats:bold> acts as a <jats:italic>tris<\/jats:italic>\u2010monodentate ligand towards three {Ni<jats:sup>II<\/jats:sup>(valpn)Ln<jats:sup>III<\/jats:sup>} binuclear nodes leading to heterotrimetallic 2D networks. The ferromagnetic interaction through the diphenoxo bridge in the Cu<jats:sup>II<\/jats:sup>\uf8ffLn<jats:sup>III<\/jats:sup> (<jats:bold>1<\/jats:bold>\u2013<jats:bold>3<\/jats:bold>) and Ni<jats:sup>II<\/jats:sup>\uf8ffLn<jats:sup>III<\/jats:sup> (<jats:bold>5<\/jats:bold>\u2013<jats:bold>7<\/jats:bold>) units, as well as through the single cyanide bridge between the Fe<jats:sup>III<\/jats:sup> and either Ni<jats:sup>II<\/jats:sup> (<jats:bold>5<\/jats:bold>\u2013<jats:bold>7<\/jats:bold>) or Cu<jats:sup>II<\/jats:sup> (<jats:bold>4<\/jats:bold>) account for the overall ferromagnetic behavior observed in <jats:bold>1<\/jats:bold>\u2013<jats:bold>7<\/jats:bold>. DFT\u2010type calculations were performed to substantiate the magnetic interactions in <jats:bold>1<\/jats:bold>, <jats:bold>4<\/jats:bold>, and <jats:bold>5<\/jats:bold>. Interestingly, compound <jats:bold>6<\/jats:bold> exhibits slow relaxation of the magnetization with maxima of the out\u2010of\u2010phase ac signals below 4.0\u2005K in the lack of a dc field, the values of the pre\u2010exponential factor (<jats:italic>\u03c4<\/jats:italic><jats:sub>o<\/jats:sub>) and energy barrier (<jats:italic>E<\/jats:italic><jats:sub>a<\/jats:sub>) through the Arrhenius equation being 2.0\u00d710<jats:sup>\u221212<\/jats:sup>\u2005s and 29.1\u2005cm<jats:sup>\u22121<\/jats:sup>, respectively. In the case of <jats:bold>7<\/jats:bold>, the ferromagnetic interactions through the double phenoxo (Ni<jats:sup>II<\/jats:sup>\u2013Dy<jats:sup>III<\/jats:sup>) and single cyanide (Fe<jats:sup>III<\/jats:sup>\u2013Ni<jats:sup>II<\/jats:sup>) pathways are masked by the depopulation of the Stark levels of the Dy<jats:sup>III<\/jats:sup> ion, this feature most likely accounting for the continuous decrease of <jats:italic>\u03c7<\/jats:italic><jats:sub><jats:sc>M<\/jats:sc><\/jats:sub><jats:italic>T<\/jats:italic> upon cooling observed for this last compound.<\/jats:p>","DOI":"10.1002\/chem.201406088","type":"journal-article","created":{"date-parts":[[2015,2,20]],"date-time":"2015-02-20T03:48:18Z","timestamp":1424404098000},"page":"5429-5446","source":"Crossref","is-referenced-by-count":76,"title":["Heterotrimetallic Coordination Polymers: {Cu<sup>II<\/sup>Ln<sup>III<\/sup>Fe<sup>III<\/sup>} Chains and {Ni<sup>II<\/sup>Ln<sup>III<\/sup>Fe<sup>III<\/sup>} Layers: Synthesis, Crystal 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