Ellen Johnson Sirleaf spoke to reporters on Friday after briefing the UN Security Council on developments in her country.
Both she and her Nigerian counterpart, Olusegun Obasanjo, announced separately that talks had begun with regional bodies to arrange for Taylor's return to Liberia.
A UN-backed special court in Sierra Leone has indicted Taylor on charges of sponsoring rebels who waged a war in that country's 1990s civil conflict. He was granted political asylum by Obasanjo in August 2003 and has been living in the southeastern Nigerian city of Calabar.
Sirleaf said: "I have consulted with President Obasanjo and asked him that we and the leaders of Africa, particularly those that were involved in the arrangement that took Mr Taylor to exile, now bring this matter to closure.
"By closure, I mean that that decision should be taken that would allow Mr Taylor to have his day in court. We have also urged that ... once the African leaders decide upon that path that they ensure that Mr Taylor ... has the full right of self-defense," she added.
"Time is of the essence in this regard. Liberia's peace is fragile. There are many loyalists in our country to Mr Taylor," Sirleaf said. "Whatever decision is taken by the African leadership must ensure that the safety of the Liberian people and the stability of our nation is not undermined."
In 1989, Taylor's rebel movement, the National Patriotic Front of Liberia, launched an insurrection in Liberia which eventually brought him to power but plunged his small nation of three million people into civil war.
In the 1990s, he was accused of sponsoring the rebel Revolutionary United Front in Sierra Leone as it carried out a campaign of torture, rape and dismemberment which targeted civilians, peacekeepers and government troops.
In 2003, Nigeria sent peacekeepers to Liberia and persuaded the besieged Taylor to accept Obasanjo's offer of a safe haven to avert a bloody showdown in Monrovia.
Charles Taylor has been living in
exile in Nigeria
Since then, however, Obasanjo has come under increasing pressure from rights groups and foreign capitals to hand over Taylor to international prosecutors in Freetown, who have prepared a 17-count indictment against him.
Richard Dicker, head of the international justice programme at Human Rights Watch, said: "Now the burden is on the council to back her to the hilt in this request and to express its expectation that Nigeria will promptly comply with the formal request [for Taylor's extradition]."
"[Taylor] is a man who has been indicted by a court set up by the United Nations of which Nigeria is a member, of which Nigeria aspires to become a member of its Security Council. There is an obligation on Nigeria to comply."
In her address to the council, Sirleaf paid a tribute to the United Nations for its role in "restoring Liberia to its rightful place in the community of peaceful nations". Liberia is a founding member of the world body.
Elected in November 2005 in a country devastated by 14 years of civil war, Sirleaf, 67, is a Harvard University-educated former World Bank economist, Liberian cabinet member and senior UN administrator.