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HP benefits both Def and Sp. Def so is generally best.
But more than that, if the Pokemon has low base HP but high base defenses (ie Dusknoir, Shuckle), you're getting more of a benefit overall from the raw increase in HP anyway in terms of sheer bulk.
The exceptions to this are
- The opposite end of the spectrum, Pokemon with high HP and (relatively) low defenses (Wailord, Drifblim), will see less of a bonus from the raw HP and more from investing in defenses.
- Eviolite Pokemon. Again, varies with stats, but the higher the defenses, the higher they are after Eviolite.
Raw numbers would depend on the individual Pokemon though.
