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Helpful answers
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Feb 15, 2014 9:46 AM in response to arburnsby Niel,You can't choose the payment method on a purchase-by-purchase basis. If none of the balance has been spent, click here and ask the iTunes Store staff to put it back onto the card.
(100483)
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Feb 15, 2014 9:48 AM in response to Nielby arburns,Unfortunately, she has spent a portion of it already. Thank you though
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Feb 15, 2014 9:48 AM in response to arburnsby King_Penguin,If you have a balance on the account then that will automatically be used up first, you can't specify how purchases are charged - from http://support.apple.com/kb/HT5582 :
When making purchases, content credits are used first, followed by Gift Certificate, iTunes Card, or Allowance Account credits; your credit card or PayPal account is then charged for any remaining balance.
If you want your PayPal account to be charged then you could try gifting the item to yourself (an account's balance can't be used for gifting) - it's not something that I've tried but I think that it should work, and I assume that Paypal works for gifting (the gifting page says that a credit card needs to be on the account, and I'm not sure that means a credit card, or just a payment method other than a balance).
Gifting : http://support.apple.com/kb/HT2736