Tsvangirai told a packed Southwark Cathedral that he had one message, that "Zimbabweans must come home."
His appeal was greeted by boos and chants of "Mugabe must go."
When Tsvangirai could not be heard above the crowd, he left the pulpit for two minutes before returning to face questions.
He said: "I did not say ‘pack your bags tomorrow,’ I said ‘you should now start thinking about coming home’."
After answering several more questions briefly, he was ushered away by security guards.
Tsvangirai spoke on Saturday about his "extraordinary" working relationship with his one-time bitter enemy President Robert Mugabe in Zimbabwe’s power-sharing government.
In an interview with the Daily Telegraph, Tsvangirai also appealed to the half a million Zimbabwean exiles in Britain to return home and help rebuild their shattered nation.
Tsvangirai insisted that Mugabe — who previously tried to crush his Movement for Democratic Change (MDC) was an essential part of the country’s "transitional solution".
"Yes, I am actually surprised"
"In fact, he is an indispensable, irreplaceable part of the transition," he said.
He admitted he was surprised that he and Mugabe can meet every Monday and talk constructively about their policies.
"It is a workable relationship, surprisingly. Yes, I am actually surprised. Who would have thought that sworn opponents like us could sit down and talk about what’s good for Zimbabwe? It’s an extraordinary experience."
In an appeal that he is expected to repeat later on Saturday in a speech in London, Tsvangirai said it was time for the men and women who fled Zimbabwe under Mugabe’s rule to return as the nation picks itself off the floor.
"The government needs these professionals. We also need whatever savings they made to help economic development. It is time to come home," he said.
"We need support if we are to avoid sliding back"
The British capital is the latest stop on a tour which has taken in Washington, Berlin, Stockholm and Brussels as he drums up support for the ‘new’ Zimbabwe — albeit one that still has 85-year-old Mugabe as president.
"We need support if we are to avoid sliding back to where we were. I am telling these leaders that I need to re-establish Zimbabwe’s relations with the outside world — we must be part of the community of nations again and not a pariah state," Tsvangirai said.
"Look at what we have achieved in the four months of this coalition government. We have brought inflation down from 500 billion percent to three percent, we have started opening schools that had been closed for more than a year, and we have reopened hospitals."
The Telegraph said the only time that the ebullient Tsvangirai’s mood darkened was when he talked about the death of his wife Susan in a car accident in March which he himself survived.
Despite immediate suspicions that it was an assassination, Tsvangirai insisted "it was an accident".
"It was a terrible experience. Susan and I had gone through all the trials, the tribulations and the triumphs and she would have loved to have seen this new Zimbabwe.
"There was a great outpouring of grief from the people of Zimbabwe when she died and in many ways her death united Zimbabweans."