To do an eye-roll, swing your eyes upward.
That's the basic action, but let's break it down for a more convincing (or subtle!) eye-roll:
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The Swing: Deliberately move your gaze upward. The key is to slightly expose more of the whites of your eyes (the sclera) above the iris. The amount you expose determines the intensity of the eye-roll.
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Arcing Motion: Ideally, the eye movement isn't just straight up. Try a slight arc - moving your eyes from one side to the other as you roll them upward. This makes the "rolling" effect more visible.
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Control is Key: A subtle eye-roll is more effective than an over-the-top, theatrical one in most situations. Practice in front of a mirror to control the speed and amount of eye movement.
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Adding Facial Expression: A slight downturn of the corners of your mouth, a barely perceptible sigh, or a raise of one eyebrow can amplify the message of your eye-roll. Be careful not to overdo it!
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Context Matters: The effectiveness of an eye-roll depends heavily on the situation and your relationship with the person you're eye-rolling at (or about!). Know your audience.
Essentially, you're conveying exasperation, disbelief, or disapproval nonverbally by subtly shifting your gaze and, potentially, accompanying it with minor facial expressions.