Single crystals of two novel tetragonal chiral materials, A(TiO)Cu-4(PO4)(4) (A = Ba, Sr), were grown from Na2Mo2O7 flux, and their crystal and chiral domain structures were characterized. Polarized-light microscopy studies of the chiral domain structures in the crystals show that Ba(TiO)Cu-4(PO4)(4) mostly hosts a multidomain state, while a monodomain state predominantly appears in Sr(TiO)Cu-4(PO4)(4). To explain this striking difference, we quantified the chirality strength of these materials by comparing atomic positions in the chiral and nearest-achiral crystal structures, revealing larger chirality strength in Sr(TiO)Cu-4(PO4)(4) than in Ba(TiO)Cu-4(PO4)(4). Our proposed mechanisms linking the chirality strength and domain formation can account for the different occurrence frequency of chiral domains in this system.