Multi-reference configuration interaction (MRCI) calculations have been employed to characterize the low-lying states of first-row transition metal dihelide dications, He(2)TM(2+) (TM = Sc-Cu). The most important state-ordering principles were determined to be the occupation of the 4s orbital and orientation of the occupied 3d orbital. The ground states of all species are predicted to be of D(infinityh) symmetry arising from a 3d(n+1) electronic configuration. For excited states with singly occupied 4s or doubly occupied 3d(sigma) orbitals, bending to C(2v) symmetry typically lowers the energy and shortens the He-TM bond length. Coupled cluster singles and doubles with a perturbative treatment of triple excitations (CCSD(T)) results for ground state spectroscopic properties are in agreement with the MRCI predicted trends.