The effective exchange integrals (J ab(M)) between two cation radicals of title compounds in the Heisenberg model were calculated by ab initio molecular orbital (MO) and density functional theory (DFT) methods, together with hybrid DFT methods. The J ab(D) values between two dimer mono-cation radicals were also estimated assuming J ab(D) = J ab(M)/2. It is found that the spin lattice obtained by the ab initio method is square planar and linear in BEDT-TTF and BETS planes, respectively, although other previous calculations show that spin lattice in the BEDT-TTF plane is a triangular one. The J ab and overlap integrals (sab ) values by the ab initio methods were used to determine transfer integral (tab ) and Coulomb repulsion (Ucff ) parameters of the Hubbard model, which were compared with those of the previous results. Implications of the calculated results are discussed in relation to the spin-mediated mechanism for superconductivity.