Writing in The Observer on Sunday, Dr John Sentamu said that the power-sharing agreement between Mugabe's Zanu PF party and the opposition Movement for Democratic Change was "dead".
He made a passionate plea to the international community "to bring an end to the charade of power-sharing" that has enabled Mugabe to remain in office.
"The impasse within the South African-sponsored negotiations between the MDC and Zanu PF has been sustained by a Mugabe regime which is unwilling to give up power and refuses to recognise the rule of law," he wrote.
Dr Sentamu compared the situation in Zimbabwe to that which he faced as a dissident in Uganda under Idi Amin before neighbouring Tanzania stepped in to oust the leader from power.
"In Uganda, we were beaten, tortured, abused and hundreds were murdered, but never did we starve to death or see the level of suffering which is to be found in today's Zimbabwe," he said.
He said that Mugabe and his closest supporters must stand trial before The Hague for their crimes against the people of Zimbabwe.
His call for Mugabe's removal echoes a similar appeal from Archbishop Desmond Tutu last week for the Zimbabwean president to be removed by force if he refuses to go volutarily.
Dr Sentamu said, "The time has come for Mugabe to answer for his crimes against humanity, against his countrymen and women and for justice to be done.
"The winds of change that once brought hope to Zimbabwe and its neighbours have become a hurricane of destruction with the outbreak of cholera, destitution, starvation and systemic abuse of power by the state.
"As a country cries out for justice, we can no longer be inactive to their call. Mugabe and his henchmen must now take their rightful place in The Hague and answer for their actions.
"The time to remove them from power has come."