The 50-year-old said he wanted to concentrate on expanding his cricket academy and other business interests.
The 71-Test veteran rejoined the Australian squad as a bowling coach in 2013 and was made an assistant coach the following year.
"I'd love nothing more than to finish this stint with victory in the World T20 in India," he said in a statement late Tuesday.
McDermott's departure follows that of batting coach Michael Di Venuto who will take up the position of head coach of English county side Surrey next month.
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