Gambari has been tasked by UN Secretary-General Kofi Annan with persuading the generals who rule Burma to take what a UN spokesman called "tangible steps forward" on human rights, democratic reform and national reconciliation.
His mission, which began Thursday, comes two months after the UN Security Council put Burma's human rights situation on its agenda.
That means Burma's military government will come under closer UN scrutiny. The United States plans to introduce a resolution on Burma's human rights abuses after Gambari returns to New York.
This was the second meeting Gambari has held with Aung San Suu Kyi. He met her last May on his first trip to Burma and had hoped then that she would be released from confinement.
Instead, the generals extended her house arrest for another year. Aung San Suu Kyi has been under detention of one kind or another for most of the past 17 years.
The United States, the European Union and Secretary-General Annan have repeatedly demanded her release.
Her National League for Democracy won a landslide victory in elections in 1990, but the military, which has ruled Burma since 1962, refused to recognize the result. As part of her confinement, Aung San Suu Kyi is not allowed to receive visitors at her home nor maintain telephone contact with outsiders, even members of her own party.
Gambari held a separate meeting Saturday with party elders, one of whom, U Nyan Win, told VOA that he is encouraged that the UN Security Council is taking up Burma's human rights situation.
"The human rights issue is the most important issue for Burma because everyday, every time and everywhere, there are human rights violations occurring in Burma."
Human rights groups are calling for the release of more than 11,00 political prisoners and an end to a continuing government crackdown on minority ethnic groups.
Earlier Saturday, Gambari traveled to the military regime's new administrative capital, Naypyidaw, 400 kilometers north of Rangoon, to meet with general Than Shwe, who heads the ruling junta.
But no details of their discussions have been released. He has also met with delegates to a national convention the generals have charged with writing a new constitution as part of a so-called road map to democracy. But most Western nations and the UN have called the proceedings a sham.