Shadow secretary for Northern Ireland Vernon Coaker and shadow chief secretary to the Treasury Seema Malhotra are the newest additions to the list of now eight departures, in addition to fired Hilary Benn.
In her letter of resignation, Malhotra said that the Labour party was "hugely divided and those divisions are growing."
"I have come to believe that under your leadership we will not be able to build bridges across the party, be the strong official opposition that the country needs or reach out to voters and build confidence in Labour," the Treasury chief of nine months told Jeremy Corbyn.
Calls inside the party for a change of leadership grew louder this week after Britain voted on Thursday to quit the European Union. Jeremy Corbyn could face a vote of no confidence.
Seven shadow cabinet ministers, however, voiced their support of the embattled party leader, with shadow chancellor John McDonnell warning now was the time for the opposition to hold together.
Shadow minister for women and equalities Cat Smith reminded fellow party members that, "Labour is a democratic socialist party whose members democratically elected Jeremy Corbyn less than a year ago. MPs should respect that."
Shadow communities secretary and Labour's 2016 election coordinator Jon Trickett said he stood with the party membership. He said a petition in solidarity with the Labour leadership had been signed by 200,000 people.