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as of right now....

He is considered the most powerful of the Gray Knights so naturally I would assume that makes him more powerful than some of the best chapter librarians like Mephiston or Tigrurius?

Obviously the most powerful psyker in the Imperium is the Emperor, but let's ignore him for the purpose of this question.

It might be Tigurius, as he hasn't discovered the extent of his power yet. He keeps on doing more and more nutty things, like tap into the Hive Mind, so it's possible that he's the most powerful Librarian.

I don't think that Voldus is necessarily the most powerful, as he could be the strongest psyker in the Grey Knights but still be less powerful than some other Librarian. There may be some other psyker in the Astropaths or the Inquisition who is more powerful, too.

 Saber wrote:
He keeps on doing more and more nutty things, like tap into the Hive Mind, so it's possible that he's the most powerful Librarian.

What's this?

It's difficult to say who is the most powerful psyker since most of them have a certain specialisation. Some psyker are much more powerful than others in certain area, but not on others. Voldus is certainly one of the most powerful psyker in the Imperium and probably its foremost authority in Sanctic Daemonology, but is he the most powerful? I can't say.

Greyfax.
Whenever attempting to deny the witch Greyfax counts as having two psycher levels more than the Psyker generating the power.

That's just mean.

I don't think GW intends for this to have a diffinative answer, they could have easily made Voldus rank 4 and made him the most powerful, keeping him at rank 3, the same as Tigerus, makes me suspect they wanna keep it vague,

Between Tigres, Voidus, and others there no confirmed but definitely a bracket of top level experts in there displines.

I dunno mephiston overcame his black rage to become something....else. It sounds like he's ascended to a higher level. Not entirely sure of the implications of this but he makes blood angels uncomfortable when they're around him last i heard.

I don't know enough of the details though.

All that said they should all pale in comparison to Magnus ;P. He's not imperium though.

Agreed that the comparison of one psyker to another isn't an apples-to-apples comparison, and only tenuously comparable.

The Eldar are the ones I usually use to make that point. They're stated to be very powerful psykers in the fluff, but in a contest of blowing gak up with your brain they tend to come short against human psykers. However, they use their psychic might in a different way. They'll reach out through the strands of the future and subtly manipulate events so that you'll get your head squished by a Warboss years before you even get the opportunity to blow the Farseer's head up in a psychic showdown.

Apples to Oranges.

It's a massive simplification, and I'm not implying that all Farseers are superior to all human psykers, but it's a good example of how comparing who is the most powerful psyker doesn't quite work.