Two homochiral 2D-layered frameworks composed of a Cu2O2 core and dicyanamide (dca) linkers, [Cu((R)-hmp*)(dca)](n) (1) and [Cu((S)-hmp*)(dca)](n) (2) (hmp* = alpha-methyl-2-pyridinemethanol), have been synthesized and structurally characterized. Preliminary investigations suggest that 1 and 2 show possible ferroelectric behaviors. Magnetic studies reveal the existence of strong antiferromagnetic interactions between the Cu-II centers in both complexes. The results demonstrate that 1 and 2 are multifunctional material candidates combining ferroelectric and antiferromagnetic properties in one molecule.