The regulator said there are "indications of misconduct or mismanagement" at Believe in Magic, a charity that works with seriously and terminally ill children.
In August 2015, One Direction singer Louis Tomlinson hosted a charity ball for Believe in Magic and reportedly donated £2m to the organisation himself.
The Charity Commission said it contacted the charity's trustees in August 2016 about regulatory concerns that emerged from multiple complaints about the charity. Believe in Magic is yet to file its accounts for the financial year ending November 2015.
"An investigation has now been opened as the commission has been unable to adequately address any of its concerns with the trustees and because there are indications of misconduct or mismanagement," a statement issued by the Charity Commission said.
Believe in Magic's website says it aims to "spread magic" to the lives of seriously and terminally ill children, through once in a lifetime experiences, magical parties, professional photographs of children or babies to capture a precious memory, celebrity visits, and gifts for children in hospitals and hospices.
The most recent accounts filed by the charity show that for the financial year ending November 2014 it received £34,152, and spent £37,868.
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