CI without Hartree-Fock SCF Usually textbooks on CI takes the SCF Hartree-Fock orbitals as a starting point. Can one use the configuration interaction method starting directly from the single-particle Slater determinants avoiding the iterative procedure. This question concerns mainly small molecules like the hydrogen molecule. Do I get a high inaccuracy in this case? If yes, why? Could this inaccuracy be decreased taking into account more configurations?
If you were to perform Full CI (within a finite basis) then I don't think that it matters whether you start with SCF orbitals or some other choice.  This solution will have the lowest conceivable energy no matter what.

But if you are doing truncated (less than full) CI, then you are very much at the mercy of your starting orbitals. In general, one would want to start with orbitals that resemble those of the actual state that you are trying to describe via CI.

Otherwise, your precious excitations (singles and doubles) may be consumed correcting the "slop" that you provided, rather than moving toward the full CI limit.