According to reports, Arthur's decision has to do with his difference with skipper Greame Smith. Arthur's resignation comes days before team's departure for India where they are scheduled to play Test and one-day series.
Corrie van Zyl, Performance Manager at the Centre for Excellence in Pretoria, is expected to be appointed as caretaker coach of the team, which leaves for India on Saturday.
Cricket South Africa (CSA) are yet to issue a statement. Arthur and CSA management reportedly held an emergency meeting here last week, to discuss the team's struggles in the Test series against England.
The three-match series ended in a draw with both the teams winning one game each. Reports say Arthur apparently met CSA Chief Executive Gerald Majola about his severance package.