Sylvia Chew, who joined Reading Council in July, had her contract terminated over what the council described as "serious concerns" with her performance.
She had previously held senior posts within children's services at Kingston Council, and before that, Haringey Council.
A statement issued by Reading Council said: "Conditions of service which apply to all senior council officers state they are expected to make significant achievements in implementing the council's targets and programmes, with progress reviewed at regular intervals.
"Following an internal review, the council has decided not to continue with the contract due to serious concerns about performance.
"The decision in no way reflects the valuable and important work being carried out by our staff on a day-to-day basis."
The council has also terminated the temporary contract of Raj Bharkhada, who was interim head of children's services. It has appointed Wendy Fabbro as interim director of children's services.
The authority is yet to be inspected under Ofsted's single inspection framework for children's services.
In its most recent inspection, which took place in March 2013, the authority was rated "adequate" for child protection services. It was also rated adequate for safeguarding and looked-after children services following an inspection in February 2012.
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