>>149945633 (OP)
It's one of them. I kinda think the origin though is his greatest story of all time. I'm kinda baiting as I am not entirely sure but I want this to also be discussed alongside our favorite stories and aspects of Spider-Man.
Show that origin story to a kid or an adult or teen who somehow never heard of Spider-Man before and you'll see them react and question morality while also being presented with interesting artwork and easily understood and elegant storytelling.
The accessibility and the broad moral questions it raises are not the only aspects to the appeal. I think that the emotions and range of Peter is explored through most of the story and the only thing missing from it is a true villain and the public hatred of Spider-Man conveyed through Jonah, everything else is there.
If This Be My Destiny is prettier, is part of an arc where Peter is hounded by a lot of people and the public, and is dealing with Aunt May dying. But it reaffirms the origin only rather than iterating on it. Same with Spider-Man No More.
KLH brings in more cerebral aspects that also question Peter's psyche by now showing how MJ is in danger putting extra pressure on him and the conflict he has with his desire to simply kill Vermin and Kraven in the form of the spider.
So yeah KLH I think is tied with the origin in my desire to read it over or in my appreciation. Night Gwen Stacy Died is a close second. Child Within and Issue 200 of Spec are also pretty close.