Here's a costume sketch by Robert Fletcher for Spock in Star Trek: TMP.
Here's a behind the scenes shot of Leonard Nimoy in make-up as he directs Star Trek III: The Search for Spock.
Next we have a series of negatives of publicity stills featuring Jane Wyatt as Amanda and Leonard Nimoy as Spock in Star Trek IV: The Voyage Home. I was so glad the filmmakers were able to bring back Jane Wyatt to reprise her TOS role. Having that continuity really did make Vulcan seem like Spock's home.
Finally, here is a series of negatives featuring shots of Leonard Nimoy preparing to film on the Klingon bridge in Star Trek IV: The Voyage Home.
The next installment of my coverage of the Roddenberry Vault will jump nearly 100 years into the future with Star Trek: The Next Generation.