Writing in the Times Ephraim Mirvis said the overwhelming majority of Britain's Jews were "gripped with anxiety" ahead of the General Election on 12 December.
"A new poison - sanctioned from the top - has taken root in the Labour Party," he said.
"How complicit in prejudice would a leader of Her Majesty's opposition have to be to be considered unfit for office?"
Giving his backing to the Jewish leader, writing on social media Justin Welby said: "That the Chief Rabbi should be compelled to make such an unprecedented statement at this time ought to alert us to the deep sense of insecurity and fear felt by many British Jews.
"Everyone in our country is entitled to feel safe and secure. They should be able to live in accordance with their beliefs and freely express their culture and faith."
Speaking at the launch of the Labour Party Race and Faith Manifesto, Jeremy Corbyn didn't address the criticism from the Chief Rabbi but did state that Labour does not tolerate anti-Semitism "in any form whatsoever".
He also made an open offer to work with the Chief Rabbi, the Archbishop of Canterbury or any other faith leader on the concerns from within their communities.
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