Google Chrome added an unnecessary popup when you add a bookmark, hiding options to edit the bookmark or delete if it was accidental (a common case for me) behind an extra click.

No, clicking the bookmark button again doesn't un-bookmark it, it just closes the popup.

I'm not sure what purpose this popup is supposed to serve. To clear confusion if the bookmark was indeed saved when you clicked the button? Was it really a problem? Never seen anyone confused with the old behavior.