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“Jody was only a little boy, ten years old, with hair like dusty yellow grass and with shy polite gray eyes, with a mouth that worked when he thought.” (Steinbeck, 4) -The Red Pony

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Work here is used in the general sense of move or shape. The boy is fidgeting with his mouth—biting or pursing his lips, or moving his tongue absentmindedly—while he thinks.

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Or possibly silently mouthing the words he is thinking. –  Janus Bahs Jacquet Sep 11 '13 at 7:05
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