The meeting came as Iran, Russia and Turkey held a summit in the Black Sea resort of Sochi, pressing their diplomatic dash to resolve Syria's six-year conflict with a new round of UN-brokered peace talks set to open in Geneva next Tuesday.
Russian President Vladimir Putin said he and Turkish counterpart Recep Tayyip Erdogan and Iran's Hassan Rouhani had agreed to a "congress" of Syrian regime and opposition forces in Sochi, aimed at boosting the Geneva process.
De Mistura said the goal was to give momentum to next week's talks in Geneva by forging a unified opposition delegation, as long demanded by the Syrian government.
He said he would travel to Moscow on Thursday for talks with Russian officials.
"I'm always optimistic... especially in this moment," he said.
The 140 or so delegates from a wide range of opposition platforms are under heavy pressure to row back on some of their more radical demands after a series of recent battlefield victories that have given President Bashar al- Assad's regime the upper hand.
Among them is Riad Hijab, who stepped down as leader of the Saudi-backed opposition High Negotiations Committee (HNC) ahead of the meeting complaining that there were "attempts to lower the ceiling of the revolution and prolong the regime".
Multiple rounds of talks hosted by the UN have failed to bring an end to the war in Syria, which has killed more than 330,000 people since 2011 and forced millions from their homes.
Factions opposed to Assad have been plagued by divisions throughout the maelstrom.
Participants in the Riyadh meeting include members of the Istanbul-based National Coalition as well as of rival Cairo- and Moscow-based groups seen as more favourable to the regime, and independent figures.
The National Coalition meanwhile said Jamil had pulled out after "disagreement over an article on Bashar al-Assad stepping down and the start of a transitional phase" in Syria.
Russian Foreign Minister Sergei Lavrov said he expected that the withdrawal of Hijab and other hardliners in recent days would "help the Syria-based and foreign-based opposition unite on a constructive basis".
Observers said it could clear the way for a new negotiating team that would water down some of the opposition's longstanding demands, notably Assad's immediate ouster.
"The Saudi pitch to the Syrian opposition has been that denial will only make the situation worse, and that they have to rethink their strategy," said Hassan Hassan, a fellow at the Tahrir Institute for Middle East Policy in Washington.
"The problem... is that the political opposition does not see it that way, and most activists are still struck in the 2012 thinking, that Assad has to be toppled."
Ahead of the meeting, dozens of prominent civilian and armed opposition figures appealed to participants not to compromise on the "ouster of Bashar al-Assad and his gang".
HNC member Yehya al-Aridi acknowledged some participants, notably the Moscow platform, were more flexible on the president's future.
But they "do not represent the choices of the revolution or the Syrian people," Aridi told AFP.
And Hisham Marwah, another National Coalition member, said his group's "positions toward Assad have not changed".
"Whoever is betting on the Riyadh conference to legitimise the presence of Assad is delusional," Marwah told AFP.
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