When the Von Trapp kids play catch with the baroness, the baroness gets hit in the crotch with a ball.
"Reverend Mother, I have sinned..."
After the Captain asks Maria why she still has her dress if all her clothes were given to the poor: "The poor didn't want this one..."
In the same scene: "Were you this much trouble at the Abbey?" "Oh, much more, sir."
"I am not finished yet!" "Oh yes YOU ARE, CAPTAIN... Fraulein."
Earlier, "I won't have to whistle for them, Reverend Captain—I mean—"
"...and THESE... are my children."
"Fraulein, is it to be at every meal, or merely at dinnertime, that you intend on leading us all through this rare and wonderful new world of... indigestion?" "Oh, they're all right, Captain. They're just happy..." (cue mass bawling)
Kurt asking Brigitta not to call Maria's dress the ugliest one they ever saw, since one of their previous governesses wore an even uglier one.
"Will father approve of this?" "Of course [...] Don't you trust me?" "No." "Smart girl."
"So long! Farewell! Au revoir! Auf wiedersehn!" "I'd like to stay and taste my first champagne! Yes?" "No." Followed by what can only be described as a :( on Liesl's face.
"...Excuse me, sir. I don't know your signal."
"You know how Sister Berthe always makes me kiss the floor after we've had a disagreement? Well, lately I've taken to kissing the floor when I see her coming just to save time."
"Hello! Here I am!" "..." "I'm from the convent- I'm the new governess, Captain." "And I'm the old butler, Fraulein."
Maria stops in the middle of her own musical number when she sees the size of the house. Julie Andrews's delivery of "Oh help" is priceless.
After Liesl casually mentions Louisa carrying a jar of spiders in her hair, Maria reacts brilliantly. And despite having a heart-to-heart with Liesl, she spends the rest of the scene sneakily checking under her bed clothes for anything. She jumps when she does find something...but it turns out to be a slipper.