Follow peace with all men, and holiness, without which no man shall see the Lord:
Well if you consider that God was interacting with them directly, even as far as walking with Adam in the garden, then yes I would consider them so as God requires Holiness before him. But they were sanctified(cleansed) by God's Holiness, not their own. This is why it is stated in scripture by John "When we see him, we will be like him..any one who has this hope in him will be pure..even as he is pure." God's presence in our lives is what makes us Holy, even though we are still in these imperfect fleshy forms.
So we have to be careful though with the word Holiness, as it doesn't necessarily denote omniscience or omnipotence, or knowledge. Remember, food and temples were considered "holy" and "sacred" by God..but these things are just objects which are not infallible or unbreakable.
All of this being said, despite the Holiness God had given them, they did not possess knowledge of good and evil. They would have remained Holy if they had listened to God, and not disobeyed his command to eat from the tree of knowledge...as God stated they would die after eating from it. God holds them accountable for this disobedience because they possessed enough knowledge from him to refrain from disobeying his command.