Two novel and fascinating high-nuclearity lanthanide-transition (4f-3d) heterometallic clusters were obtained based on an anion-template (Cl-) and ligand-controlled approach, formulated as [Gd40Ni44(CO3)(12)(CH3COO)(4)(IDA)(44)(C2O4)(mu(2)-O)(4)(mu(3)-OH)(60)(mu(3)-O)(6)(H2O)(12)]center dot Cl-10 center dot 20H(2)O (abbreviated as Gd40Ni44, 1) and [Eu40Ni44(CO3)(12)(CH3COO)(6)(IDA)(44)(C2O4)(mu(2)-O)(4)(mu(3)-OH)(62)(mu(3)-O)(4)(H2O)(12)]center dot Cl-10 center dot 23H(2)O (abbreviated as Eu40Ni44, 2), where H(2)IDA = iminodiacetic acid and H2C2O4 = oxalic acid. Structural analysis exhibits that the compounds 1 and 2 were both constructed by two enticing bowl-like anion units Ln(20)Ni(22), featuring peanut-like structures. Besides, the assembly of Ln(20)Ni(22) was templated by five Cl- ions. Magnetically, compound 1 shows a significant magnetocaloric effect, with -Delta S-m = 36.05 J kg(-1) K-1 at 3 K for Delta H = 7 T.