Another two of my favorite Steve moments was in the "Dinosaurs" episode, "Into the Woods." The way he was puppeteering Blarney cracked me up. Then there was the character he did named Woody, which was basically him using the Wembley voice, sure, but waaaaaaaayyyyyy more hyperactive.
Oh my garsh, I forgot about Blarney! Lol. Speaking of Dinosaurs, they just put it on Hulu, so i'm gonna definitely watch that today.
If we're going by favorite Steve moments overall and not just Muppets:
SST: The sketch where Ernie sings "Wake Up", Steve's energy in this is just so infectious. Also the "Lights, Camera, Bert!" episode where his comedic timing is spot on as well as his chemistry with Eric. I also thought he was really funny in those Dr. Feel sketches.
Fraggle Rock: Basically any episode about Wembley, and all of the scenes with Doc and Sprocket.
Dinosaurs: The above mentioned Blarney cameo.
Muppets: Bean Bunny in Muppets Christmas Carol.
His performance as Kermit in The Muppets (2011) was really the first time I excepted him as not just an imitator of Jim.
Also, his performances as Kermit on the TV show. Now, I know the writing for him in it wasn't always great, but I feel like this was Steve at the top of his game. Kermit really felt like a real breathing actor in it. And the ways Kermit emoted, Steve's hand must've been getting contorted in all sorts of unnatural ways. It was amazing. He definitely deserved in Emmy.
Least favorite: Kermit's depression in that TV Christmas movie.