The Movement for Democratic Change says its leader Morgan Tsvangirai beat President Robert Mugabe in the March 29 vote, and initial results showed it had also ended the ruling party's 28-year hold on parliament.
A delay to the presidential result and a recount of some parliamentary votes has brought growing international pressure on Mugabe, 84, and stoked fears of bloodshed in a country already suffering an economic collapse.
Dozens of riot police detained around 100 MDC supporters who were taken away in a crowded police bus, a Reuters witness said. The MDC said 200 to 250 police took part in the raid and they also took away computers used by the election command centre.
"These armed police have taken hundreds of people that were now staying at the party headquarters running away from the different parts of Zimbabwe, where the regime has been unleashing brutal violence," an MDC statement said.
Spokesman Nelson Chamisa said "They are trying to destroy evidence of their brutality."
Police said the raid targeted people who had sought refuge with the opposition after committing crimes outside Harare.
"Some of them are not office workers at all. We are busy screening them. There are some cases we are investigating and we will release those who have not committed any crime," said police spokesman Wayne Bvudzijena said.
"MYOPIC STOOGES"
Mugabe, a hero of the struggle for independence, accuses the opposition of conspiring with Western critics to bring him down.
Zimbabwe's state-run Herald newspaper on Friday called African leaders "myopic stooges" for joining the Western criticism of Zimbabwe's handling of the election.
In an unprecedented move by a region growing increasingly impatient with Mugabe, Zimbabwe's neighbours refused to let a Chinese ship unload weapons for his country amid the election deadlock. China said the ship would head home.
"The attempt to link the shipment to the post-election environment should convince sceptics of the lengths to which the Westerners and their lackeys will go to manufacture a crisis in Zimbabwe," The Herald said.
Zimbabwe's trade union federation, which is close to the opposition and was once led by Tsvangirai, said it had received reports that a second consignment of more sophisticated Chinese weapons would now be flown to the landlocked country.
The top U.S. diplomat for Africa, Assistant Secretary of State Jendayi Frazer, said on Thursday the United States backed calls from former colonial ruler Britain for an arms embargo.
But the Herald newspaper said the country needed arms to defend itself.
MDC leader Tsvangirai accuses Mugabe of delaying results to rig victory and stay in power in Zimbabwe, whose economy lies in ruins with 165,000 percent inflation and chronic food and fuel shortages.
The recount in 23 of 210 constituencies could overturn the results of the parliamentary election, which showed Mugabe's ruling ZANU-PF losing its majority for the first time.
The Zimbabwe Electoral Commission (ZEC) has recounted nine constituencies, and so far all candidates who were originally declared winners have retained their position. The full recount results were expected by the weekend.
A coalition of Zimbabwean church groups on Friday called on the ZEC to "release the true results" of the election, and urged African countries and the United Nations to help end the crisis.
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