The 26 bishops should “be on the side of those who ... want a dignified, compassionate end to their lives”, Lord Carey told the Guardian.
Carey, who retired as head of the C of E in 2002 and still sits in the Lords, said he would back Kim Leadbeater's bill to legalise assisted dying "because it is necessary, compassionate and principled".
He said it was "ironic that I will represent the vast majority of Anglicans who favour change, and the bishops in the House of Lords will not".
Carey's position is in contrast to that of the current archbishop of Canterbury, Justin Welby, who this week described Leadbeater's bill as dangerous, saying it could put people under pressure to ask for an assisted death.
Stephen Cottrell, the archbishop of York, also said the state "should not legalise assisted suicide", saying better provision of palliative care was the right response to end-of-life suffering.
Alan Smith, the bishop of St Albans and convener of bishops sitting in the Lords, said: "In the past, bishops have consistently opposed legislation to introduce assisted dying/suicide. It is likely that we will do the same in the future."
According to the Rev Canon Rosie Harper, a former member of the General Synod, the C of E's ruling body: "There is a real disconnect between the [church] hierarchy and what people in the pews think. And I suspect there's a disconnect between what bishops feel they have to say and what many of them actually think."
Opinion polls have shown support for assisted dying among church-goers is roughly in line with the 65%-75% of the general population that backs a change in the law. A survey of clergy by the Times last year found that more than a third of priests in the C of E backed assisted dying, up from 22% in 2014.
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