Yes, you can modify the count of an element in a Python Counter by directly assigning a new value to it. For example, if you have a Counter c with elements {'apple': 2, 'banana': 3}, and you want to change the count of 'apple' to 5, you can do c['apple'] = 5. This will update the count of 'apple' to 5 on the Counter. Keep in mind that if you assign a count of 0 to an element, it will effectively remove that element from the Counter.