The McCune Foundation was established in 1979 by the will of Charles L. McCune. The donor, a Director of The Union National Bank of Pittsburgh for 56 years, served as its President from 1945 until 1972, and then as Chairman until his death. During his life, Charles McCune gave generously to charitable organizations, mostly in the Pittsburgh area, while seeking no public recognition of his philanthropy. He established the Foundation in memory of his parents, Janet Lockhart McCune and John Robison McCune.

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In the donor's will, it was stipulated that all Foundation assets had to be distributed prior to October 16, 2029 (50 years after his death). In 2012, McCune Foundation, as part of its "sunset" strategy, made the decision to focus its grantmaking efforts on qualified beneficiaries located in the following western Pennsylvania counties: Allegheny, Armstrong, Beaver, Bedford, Blair, Butler, Cambria, Fayette, Greene, Indiana, Lawrence, Somerset, Washington and Westmoreland. More information on grantmaking guidelines and a map of granting areas can be viewed under the Grants tab.