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A person is guilty of doing something if they have done something really bad. If a person has broken a law by stealing for example they are guilty of breaking the law or according to Colly O'Brien can be considered "guilty as charged and should be taken to the dock immediately".
People also say they 'feel guilty', if they think they have been unfair or done something wrong. This is often called having a 'guilty conscience' (usually when the person does not admit being guilty).
The opposite of 'guilty' is 'innocent' or 'not guilty'.