He has been held in Turkey for two years and accused by local prosecutors of "terrorist" ties to the Islamist Gulen movement, which has been blamed for a failed coup in July 2016.
"We have more that we're planning to do if they don't release him quickly", Mnuchin said when asked by President Trump at a Cabinet meeting for an update on USA sanctions on Turkish officials. "He's not a spy".
Turkey and the United States are now experiencing rocky relations following Washington's imposition of sanctions on Interior Minister Suleyman Soylu and Justice Minister Abdulhamit Gul for not releasing American pastor Andrew Brunson, who faces terrorism charges in Turkey.
Mr Erdogan wrote in the New York Times earlier that unless the USA changed course, Turkey would look for new friends and allies.
Qatar defied US President Donald Trump on Wednesday and promised to plough $15 billion into Turkish financial markets and banks.
The currency has lost almost 40 percent against the dollar this year, driven by worries over Erdogan's growing influence on the economy and his repeated calls for lower interest rates despite high inflation.
U.S. sanctions and tariffs have contributed to a tumble in the Turkish lira, which dropped in value to 5.86 to the dollar on Friday following Mnuchin's warning.
The pastor row is one of several between the North Atlantic Treaty Organisation allies, including diverging interests in Syria and U.S. objections to Ankara's ambition to buy Russian defence systems, that have contributed to instability in Turkish financial markets.
JP Morgan said moves by Turkish authorities showed they were committed to stabilising the currency with technical measures such as restricting foreign exchange swaps and cancelling repo auctions to push up the average cost of bank funding.
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Finance Minister Berat Albayrak assured worldwide investors on Thursday that Turkey would emerge stronger from its currency crisis, insisting its banks were healthy and signalling it could ride out the dispute with the United States.
Turkey has proven a key ally for Qatar over the past year, helping the tiny Gulf nation ride out a more than 14-month blockade by its powerful neighbors, including Saudi Arabia, with which it shares its only land border.
Tamim bin Hamad Al Thani, the Amir of Qatar, tweeted: "Today, in the framework of important negotiations with His Excellency President Erdogan in Ankara, we announced a package of deposits and investment projects worth $15 billion in this country, which has a productive, strong and robust economy".
Brunson, an Evangelical pastor residing in the coastal province of Izmir, is standing trial in Turkey over terrorism charges.
Mr Trump described him as "our wonderful Christian Pastor, who I must now ask to represent our Country as a great patriot hostage".
Last week, the U.S. doubled its tariffs on metal imports from Turkey.
U.S. Treasury chief Steve Mnuchin earlier said the U.S. could put more sanctions on Turkey. The lira's sharp decline has sparked fears in the global community of a Turkish economic crisis.
The unnamed source added that they had agreed that their finance ministers - Berat Albayrak and Bruno Le Maire - would meet "as soon as possible", and that Mr Macron had told Mr Erdogan that Turkey's economic stability was "important" for France.
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