Two homochiral MOFs, (CBQ)CuI3(CN)3Br (1) and (CBC)CuI2.5(CN)2Br1.5 (2), were prepared by the solvothermal reaction of CuCN with N-4-cyanobenzyl quinidinium bromide (CBQ-Br) and N-4-cyanobenzylcinchonidinium bromide (CBC-Br). 1 and 2 are typical ferroelectric compounds while may have dipolar relaxation ferroelectrics and a high dielectric constant (epsilon o = 119.3).