I also liked some of the Unique Weapons in Fallout 3, thus http://www.fallout3nexus.com/downloads/file.php?id=1296 was created by me because of the weapons lack of personality, or rather it's ability to shine.
So now I'm finding myself wishing something similar for unique NPC robots, there are a few singular mods such as The Megaton Deputies, which rocks my face, but a compliation of these mods would be wicked.
So, I'll throw some ideas for each of the unique robots and unique textures/meshes for them.
Deputy Weld/Deputy Steele: The Megaton Deputy mod is a great start; badges, cowboy hats, etc. That alone is perfect
Wadsworth/Godfrey: Some sort of tuxedo/butler-ish texture would suit them well
Nuka-Cola Plant Foreman: A Nuka-Cola Paint Job
Shakes: Oh what glee I'd have to have this particular Protectron textured with a bartender paint job. And a little bowtie Such, such glee.
Dean Dewey: A professors tan suitcoat paint job and a name tag would be awesome. And a monocle. Oh yes.
RL-3: A Black-Ops Color Scheme with Red Eyes, and a patch to make it compatible with major follower mods (Phalanx, etc)
Mister Buckingham: A bell hop color scheme, and a bell hop's hat.
Andy: A Vault 101 Color Scheme, for sure
So... yeah. My idea. Woo.