HMV went into administration last month, putting more than 4,000 jobs at risk, although it continues to trade all its 220 stores.
Nick Edwards, joint administrator at Deloitte, said it has decided to close the 66 stores to "enhance the prospects of securing the business' future as a going concern".
"We continue to receive strong support from staff and are extremely grateful to them for their commitment during an understandably difficult period. All other key stakeholders remain very supportive and I continue to be hopeful of securing a future for the restructured business."
Last week 190 jobs were cut in HMV's head office and distribution centre.
