disobedience toward God: the refusal to be won over by what he has said, which is at once a refusal to obey it and a refusal to believe it
This is the noun that goes with the verb "to disobey" (ἀπειθέω), and both are built on the ordinary Greek word for being persuaded, with a prefix that cancels it. So the word does not first mean breaking a rule. It means refusing to be won over: God has spoken, the case has been made, and a person will not yield.
Because of that, it sits exactly where disobedience and unbelief overlap. The writer of Hebrews uses it of the wilderness generation who never entered God's rest, and two verses earlier he calls the very same failure by the plain word for unbelief (ἀπιστία) in Hebrews 3:19. Paul uses it of everyone alike: God has shut all people up in this refusal so that he can show mercy to all.
Paul's letters also use it in a fixed phrase, "the sons of disobedience." That is a Hebrew way of naming what someone belongs to rather than who their father was, much as "son of peace" means a peaceable person. It describes a settled way of living, an allegiance, not a single lapse.