Dr John Sentamu urged people to offer prayer, money and practical support as part of the effort.
"I am inviting people to work with me for the restoration of Zimbabwe in order that peace, prosperity and the rule of law are restored to that once great and prosperous land of hope for Africa which has become a waste land of oppression, poverty and disease," he said.
The Archbishop made the appeal as he announced a special service for the people of Zimabwe, to be held at the historic St Margaret's Church in Westminster on Friday 11 July.
'Restore-Zim' has been organised in conjunction with Westminster Abbey to support troubled Zimbabwe and its people as they continue to face economic, political and social turmoil.
Dr Sentamu has been a fierce critic of Zimbabwe President Robert Mugabe. Last December, the Archbishop made headlines when he cut up his clerical collar during a television interview, vowing that he would not wear one again until Mugabe is ousted from power.
In a statement on Tuesday, Dr Sentamu appealed to the British public to live up to their reputation for compassion by speaking out on Zimbabwe.
"People from Britain have a proud record of making a difference in the lives of people around the world. Whether it be the anti-apartheid movement, the ending of Ian Smith's UDI, the Jubilee Debt Campaign or countless other campaigns, British men and women have shown how their compassion and outrage over injustice can be channelled positively into bringing about new life and new hope," he said.
"This is an opportunity for civil society to engage - not by proxy through Government - but as ordinary British citizens joining their voices together with those from Africa to form a chorus calling for restoration in Zimbabwe and an end to the brutalisation of its people."
Dr Sentamu said the campaign for Zimbabwe's restoration was not a party political venture.
"It is not pro-MDC or anti-Zanu PF. Rather it is for the people of Zimbabwe, black and white, being helped by those here in Britain, white and black," he said.
"We need to remember there is only one race - the human race - and in joining together to restore Zimbabwe, we ease the sufferings of our brothers and sisters."
Dr Sentamu's call came as opposition leader Morgan Tsvangirai ruled out on Wednesday the possibility of talks on a power-sharing government until President Mugabe puts a stop to violence against MDC leaders and supporters and declares him as the rightful election winner.
Tsvangirai won the first round of the presidential election in March but pulled out of the June 27 run-off because of attacks on his supporters.
