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A new hydrazone Schiff base bridging ligand (H₂L_Schiff (<i>E</i>)-<i>N</i>′-((1-hydroxynaphthalen-2-yl)methylene)pyrazine-2-carbohydrazide) and <i>L</i>/<i>D</i>-proline were used to construct a pair of homochiral Dy₆ cluster complexes, [Dy₆(CO₃)(<i>L</i>-Pro)₆(L_Schiff)₄(HL_Schiff)₂]·5DMA·2H₂O (<i>L</i>-<b>1</b>, <i>L</i>-HPro = <i>L</i>-proline; DMA = <i>N</i>,<i>N</i>-dimethylacetamide) and [Dy₆(CO₃)(<i>D</i>-Pro)₆(L_Schiff)₄(HL_Schiff)₂]·5DMA·2H₂O (<i>D</i>-<b>1</b>, <i>D</i>-HPro = <i>D</i>-proline), which show a novel triangular Dy₆ topology. Notably, the fixation of CO₂ in the air formed a carbonato central bridge, playing a key role in assembling <i>L</i>-<b>1</b>/<i>D</i>-<b>1</b>. Magnetic measurements revealed that <i>L</i>-<b>1</b>/<i>D</i>-<b>1</b> displays intramolecular ferromagnetic coupling and magnetic relaxation behaviours. Furthermore, <i>L</i>-<b>1</b>/<i>D</i>-<b>1</b> shows a distinct magneto-optical Faraday effect and has a second harmonic generation (SHG) response (1.0 × KDP) at room temperature. The results show that the immobilization of CO₂ provides a novel pathway for homochiral multifunctional 4f cluster complexes.