Mugabe must "exit from active politics in Zimbabwe," said Morgan Tsvangirai, head of the Movement for Democratic Change (MDC), in a statement.
He said the MDC, formed four years ago, "welcomes and fervently supports all regional, continental and international efforts to chart a peaceful course towards the resolution of the crisis of governance in Zimbabwe".
His comments came days before a high-profile visit to Africa by US President George W Bush, and an African Union summit in neighbouring Mozambique.
Earlier the MDC said it was sending its officials to South Africa and Mozambique to lobby international leaders on the situation in Zimbabwe.
US Secretary of State Colin Powell has called on Mugabe to leave office and said the subject of Zimbabwe will be high on the agenda during Bush's July 8-9 visit to South Africa.
Tsvangirai called for resumption of dialogue between his party and the ruling Zimbabwe African National Union - Patriotic Front (ZANU-PF).
He made a series of demands, including restoration of the rule of law, the removal of strict press and security laws and an end to what he termed "state-sponsored violence".
"It is in the context of this demonstration of sincerity by the regime that dialogue can meaningfully begin," the MDC leader said.
Tsvangirai has rejected Mugabe's victory in last year's disputed presidential poll.
The opposition party blames the government for severe social and economic hardships as well as political tensions gripping the country. - Sapa-AFP.
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