Might just be me, but it's pretty amusing when Morgoth and Ungoliant get into their argument. Ungoliant tells Morgoth that, for her help, she wants to eat the world. Morgoth basically replies "You can't eat the world, I have to rule it!"
Beren tries to hold off Carcaroth with a Silmaril in his hand. Carcaroth responds by eating Beren's hand. Om nom.
Beren pronounces, "Even now a Silmaril is in my hand." He subsequently holds up his bloody stump of where his hand used to be.
Haleth cracking the only joke in the whole book, and it's actually a pretty good one, if rather dark. Bascially, 'If Thingol thinks I'm going to join up with Melkor after what he did to my family and my people, then the minds of Elves are strange, scary places.'