Ian Thomas, who took over as director of children's services in Rotherham in January 2015, will become chief executive of Lewisham Council.
The news comes little more than a month after children's services in Rotherham were rated "good" by Ofsted, three years after being judged "inadequate".
Rotherham Council said deputy strategic director Mel Meggs will step into the post in an acting capacity when Thomas leaves, while the council seeks to recruit a permanent replacement.
Chief executive of Rotherham Council Sharon Kemp said: "Ian has led children's services through their improvement and has achieved many changes, taking them from being rated as inadequate by Ofsted three years ago to the recent overall good rating, with outstanding features.
"He leaves the service and the council in a very good place and we are confident this will enable us to seek a replacement of equal calibre as quickly as we can."
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