Four kite-like tetranuclear Zn(II)Ln(III)3 (Ln= Gd 1, Tb 2, Dy 3, Ho 4) clusters supported by p-tert-butylthiacalix[4]arene (H4BTC4A) have been prepared under solvothermal conditions and structurally characterized by single crystal X-ray diffraction and powder X-ray diffraction (PXRD). In the structures of these four complexes, each of them is capped by two tail-to-tail p-tert-butylthiacalix[4]arene molecules to form a bent sandwich-like unit. The photoluminescent analyses reveal that the H4BTC4A is an efficient sensitizer for Tb(3+) ions in 2. The magnetic properties of complexes 1-4 are also investigated, in which complex 3 exhibits slow magnetization relaxation typical for single molecule magnets.