Two scenes in The Wizard of Oz:
1. During the tornado, Dorothy looks out of the window and sees Miss Gulch riding her bike. Miss Gulch gets swept up in the air and turns into the witch.
2. At the witch's castle, Dorothy looks into the crystal ball and sees Aunty Em crying. Suddenly she'd replaced by the witch, laughing, and the witch's face fills the whole screen.
Also the scene in 101 Dalmations (the original animation) when Cruella de Ville puts down the newspaper and you see her laughing evilly. Again, her face fills the whole screen.