No. PS3 and PSP have separate PlayStation Network wallets, even if signed in with the same account. Funds added on one device do not automatically transfer.
To Add Funds on PSP
On PSP, go to PlayStation Network → Account Management → Add Funds.
Choose credit/debit card, PayPal, or a PSP-specific PSN card (same codes work, but redemption must happen on the PSP or via web store while PSP is primary).
Alternatively, use the PlayStation Store website on PC, set PSP as “Download to” device after purchase.
Wallet balances are per-device-family (PS3/PSVita share; PSP is separate legacy system).