Whether you can use the card elsewhere is not particularly relevant, different stores have different rules for what they will or won't accept for obvious reasons.
If it's a debit card that might be why it's being declined, not all seem to still be accepted by iTunes, and they might no longer be accepted at all in some countries.
For a card to have a chance of being accepted it needs to be registered to the same name and address (including format and spacing etc) that you have on your iTunes account, and have been issued by a bank in the country where you are (and therefore the country which is on your iTunes account).