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There is no way to send back an actual SMTP bounce message, but you can send back an automated response if you really want to. Go to your Gmail Labs Settings and turn on the "Canned Responses" lab. This lets you save snippets of text, which can then be inserted into emails automatically. Create a new message, the way you normally would. Write the ...

My suggestion: create a bounce@example.com account, and suspend it. Later, add as many aliases as needed for that account. Worked like a charm for me, with the following return message: Delivery to the following recipient failed permanently: bounce@example.com Technical details of permanent failure: Google tried to deliver your message, ...

I can think of a hack which won't be a real bounce back, but might be good enough for your use case: Create another account which will bounce back emails (e.g. nouser@example.com). Create a filter in your catchall account which forwards the bad email to that account (e.g. if you want mark@example.com to be bounced back, set up the filter ...