As in most of Ecuador, you can pay by cash or by credit card in most major places, although cash is preferred at most small shops and transportation. There is a Banco de Pacifico with ATM. Depending on your banknet, it may or may not accept your bankcard. If not, walk in the bank and talk to David about a Visa advance. He's a nice guy and speaks English.
There are many souvenir shops on the Malecón Av. Charles Darwin and the surrounding side streets. Galapagos coffee is always a popular item with prices ranging from $6.50/lb for vacu-packed coffee to $15/lb if you want it in a cute tin or box. Several talented local artists have a gallery in the upstairs of Casa Blanca, also on the Malecón.
Remember, never buy handicrafts made with local natural resources, it is forbidden by the Galapagos law, it is a National Park!