Two examples of heterometallic-organic frameworks (HMOFs) composed of dicarboxyl-functionalized Fe(III)-salen complexes and d(10) metals (Zn, Cd), [Zn2(Fe-L)2(μ2-O)(H2O)2]⋅4 DMF⋅4 H2O (1) and [Cd2(Fe-L)2(μ2-O)(H2O)2]⋅2 DMF⋅H2O (2) (H4L = 1,2-cyclohexanediamino-N,N'-bis(3-methyl-5-carboxysalicylidene), have been synthesized and structurally characterized. In 1 and 2, each square-pyramidal Fe(III) atom is embedded in the [N2O2] pocket of an L(4-) anion, and these units are further bridged by a μ2-O anion to give an (Fe-L)2(μ2-O) dimer. The two carboxylate groups of each L(4-) anion bridge Zn(II) or Cd(II) atoms to afford a 3D porous HMOF. The gas sorption and magnetic properties of 1 and 2 have been studied. Remarkably, 1 and 2 show activity for the photocatalytic degradation of 2-chlorophenol (2-CP) under visible-light irradiation, which, to the best of our knowledge, is the first time that this has been observed for Fe(III)-salen-based HMOFs.