Alright, so now that the results of this poll are in, I wanna kinda go off about a thing. First of all, I went into this not knowing shit about FMA other than like... a vague bit about Nina Tucker. That said, my girlfriend and I were talking about this question before I posted it because I had said that I believe Falin's would be the most painful of the two. After this poll, I do see where some people stand, however I would like to be the crazy person here and argue why I still firmly believe Falin's transformation to be more painful to me overall.
As mentioned several times by folks in tags, Nina Tucker's situation is hopeless, it is a tragic, overwhelmingly sad, and genuinely heartbreaking situation. Nina is a child who doesn't deserve the awful ending she met. The transformation was an act of pride, greed, and absolute recklessness. However, in my opinion, at least taking into account only the initial introduction of Nina Tucker, this hopelessness is what makes it less painful. There is nothing to yearn for. Nothing to give the viewer that desperate feeling that maybe, just maybe, things will be okay.
Falin, on the other hand, is a completely different story. Hers is a story full to the brim, overflowing with hope. Starting off with a small party of friends, lovers, family, desperate to bring their loved one back. We see the lengths to which they are willing to go. Laios willingly sacrificing a limb (granted, probably knowing it was this or death), and Marcille, dear Marcille, using a magic so forbidden, she effectively condemns herself to a life in hiding, or hell even death, without so much as a second thought to bring back Falin.
So then we see this hope, this beautiful sweet loving hope, bring back Falin when all seemed nearly lost... only to have her snatched away again. This time though, it isn't a matter of "can we revive her in time?"
This time, Laios watches his sister, a shred of herself, tear through people like they're made of butter. This time, Marcille gets to watch what she created, an amalgamation of her best friend, a person she loves so dearly, and a bloodthirsty and vicious dragon that is controlled by the mad mage. This time, it's not just a matter of lack of preparation, of doing what they can and still failing. This time it's their fault... and yet, there is still hope.
Maybe they can fix this. Maybe Marcille's magic started this, but it could end it too, right? They could keep going, they could defeat everything in their path, hell, defeat the mad mage, and find a way, any way, to fix Falin and bring her back. Because despite everything, despite the failures, the setbacks, the death, the fear, the absolute hell that they've been through, they've done the impossible before. So despite all that unknown, despite the uncertainty and the insecurity that they all feel, they persist. Because they have hope.
And I don't know about you all, but to me hope is so much more painful of a knife than acceptance.