Naturally, for as long as I can remember, I've associated him with his role as Spock. As a little kid, I'd see reruns of the original Star Trek on TV, and one of the things that stood out the most was Spock providing the steady anchor onscreen against Kirk's cartoonish flamboyancy. I wasn't paying attention to the dialogue so much as the rhythm of the characters and how they navigated each story, and Spock always had his own tune. The words became more important when I came back to the series later as a teenager, and while I would tend to identify more often with other characters, Spock remained one of the ones I liked the most. He was thoughtful and smart, always did the right thing, and, because of his alien status, was always a little (or a lot) isolated from his companions. And yet, despite that rigorously logical personality and approach to life, Nimoy managed to add enough subtle touches to keep the character from being totally alien to the audience, and gave us something to like. But I think it was in the 'Trek movies of the 80s and early 90s where Nimoy most excelled in his performances, again, using his ability to add those subtleties to stand out from fellow cast members or story lines that were frequently not subtle, and to underscore just how much was going on inside Spock as he dealt with each crisis.
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Then there was the mind-meld scene with Kim Cattrall (and her horrible hair) in Star Trek VI — The Undiscovered Country. Here, Nimoy teases us with a deceptive amount of emotion: Spock is clearly angry at Valeris' betrayal, and coldly resolved to pry the information about the conspiracy out of her. And yet, for all of that, he's holding so much back because the character is holding so much back. As a Vulcan, Spock's emotions would have been explosive at that moment, but because Vulcans fight to keep their emotions in check, and Spock more than most, half the battle you see onscreen on Nimoy's face is the character's fight to keep himself under control. It makes the scene that much more frightening because as Spock forces the mind-meld and starts tearing away Valeris' mental defences and boring into her memory (and let's call a spade a spade here, what's clearly happening is a mental rape: Spock is forcing himself inside Valeris against her will), the viewer can see that Spock has reconciled himself with having to commit an atrocity against one of his proteges, an act of brutality that he will have to live with for the rest of his life (and one that won't be easy to live with, given his acceptance of the need to acknowledge some emotion, unlike other Vulcans), and who wouldn't be scared of someone who could do that — and, more importantly, do something that monstrous, reveal that ability within themselves, in front of their friends? The viewer can also see from Valeris' reaction that not only is she being painfully brutalized, but because the mind-meld allows her to fully experience Spock's consciousness, she is feeling the full force of his Vulcan rage behind his cracked facade of emotional control, and she is clearly terrified. Very few other actors could have done this without over- or under-acting.
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And maybe it's appropriate to end with The Hallowe'en Tree. As fans, while we celebrate Leonard Nimoy's life and performances, let us also say "Carry his pumpkin gently, Moundshroud. Gently."