"One thing that needs to happen is Mr. Taylor needs to leave," Bush told CNN. "I think most people understand that that's important. I'm convinced he will listen and make the right decision, if he cares about his country."
International pressure on Taylor increased after hundreds of protesters went onto the streets of the capital Monrovia Thursday, waving signs saying "Taylor must go."
Some of them also urged the U.S. to send troops. America has a special historical relationship with Liberia.
A senior Liberian government source told CNN Thursday that Washington had given Taylor 48 hours to give up power and leave, although a State Department official in Washington said he was not aware of an ultimatum.
But White House staff say urgent efforts are under way to get Taylor out, with the National Security Council discussing the issue Friday.
Taylor was indicted in June by a U.N.-backed special court in neighboring Sierra Leone on charges of perpetrating war crimes by arming and training rebels who committed atrocities in the country.
He has demanded assurance he would not have to face those charges in return for stepping down.
Nigeria has tentatively offered Taylor asylum, an offer he initially rejected. A Nigerian delegation is expected to return to Monrovia Friday, following a visit Wednesday.
Bush, who is due to visit Africa next week, said he would examine "all of the options to determine how best to bring peace and stability" to Liberia, including the possibility of sending troops as part of an international peacekeeping team.
In an interview with CNN International's "Inside Africa," the U.S. president stressed the need to get Taylor out but would not say whether U.S. troops would depose him if he refused.
The Pentagon has told U.S. European Command to prepare military options and recommend possible U.S. intervention in Liberia.
Bush told CNN that U.S. officials were holding talks with the Economic Community of West African States "to determine what the nature of a peacekeeping force might look like.
"I'm the kind of person that likes to know all the facts before I make a decision," he said.
The Liberia issue has become a test of Bush's promise to make a commitment to promoting peace, democracy and economic development in Africa.
At least 50 U.S. Marines from a unit at the U.S. Naval Station in Rota, Spain, that specializes in rapid anti-terrorism missions could arrive within six hours of receiving an order, a Marine Corps spokesman said. Sources said they would be used to reinforce the U.S. Embassy in Monrovia.
National Security Adviser Condoleezza Rice said: "Charles Taylor needs to leave because Charles Taylor is the problem -- not just a problem for Liberia, he's a problem for the region."
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