This work demonstrates a new Lindqvist-like [FeIII6(μ6-O)L4Cl6]2- (Fe6, L = 2-(hydroxymethyl)-2-(pyridin-4-yl)-1,3-propanediol) cluster for the construction of a novel class of Fe-cluster organic frameworks. The novel Fe6 cluster can be used to build not only a homometallic MOF, but also a heterometallic MOF by introducing copper halide clusters to the reaction system. In particular, the heterometallic MOF achieved a skillful combination of Fe6 SBU and cuprous-halide clusters for the first time. Our synthesis strategy opens up an effective avenue to novel Fe-cluster-based MOF materials.