1

Harry shook his head, noticing as he did so that the ache in his right temple was getting worse.

Harry Potter and the Order of the Phoenix

I feel as he did so is kind of redundant. What additional information does it add here?

2

The use of as he did so explicitly let us know that the act of shaking his head occurs simultaneously with the act of noticing. As pointed out in comments, as written by the author, the sentence could be paraphrased as:

Harry shook his head, noticing at the same time that the ache in his right temple was getting worse.

Otherwise that sentence could have been interpreted differently.

For instance:

Harry shook his head, noticing (then, later) that the ache in his right temple was getting worse.

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