Focusing on the recently-discovered candidate topological insulator α-(BEDT-TSeF)₂I₃—having two-dimensional charge-neutral Dirac cones in a low symmetry lattice—we combine ab initio and extended-Hubbard model calculations to deal with spin-orbit and nonlocal repulsive interactions, and find a realization of an interaction-induced quantum spin Hall (QSH) insulator, similar to the one proposed in the honeycomb lattice under next-nearest-neighbor repulsions. In the absence of repulsive interactions, a topological insulator appears by the spin-orbit coupling and is characterized by a nonzero spin Chern number. By considering up to next-nearest-neighbor repulsions at Hartree-Fock level, the intrinsic spin-orbit gap is found to grow by orders of magnitude and a QSH insulating phase appears that has both a finite spin Chern number and order parameter. Transport coefficients and spin susceptibility are calculated and found to consistently account for most of the experimental findings, including the metal-to-insulator crossover occurring at ∼50K as well as the Berry phase change from 0 to π under hydrostatic pressure. We argue that such a QSH insulating phase does not necessitate a sizable spin-orbit interaction to generate a large insulating gap, which is highly advantageous for the search of novel topological phases in generic materials having low symmetry lattice and/or small spin-orbit coupling.

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