A spokesman for the musician said Mrs Goulden died of natural causes after a long illness.
She helped transcribe many of Sir Cliff's songs and is known to have been an inspiration to him at the beginning of his music career.
She leaves her husband Terry and two adopted Vietnamese children, as well as Sir Cliff and their two other sisters Joan, 66, and Jacqui, 68.
Despite the news Sir Cliff performed for thousands of fans on Saturday in Denmark. They didn't know he was grieving the loss of his sister.
The singer's bereavement comes just weeks after false allegations that he sexually abused children were finally dropped after years of investigation, including a televised raid on his Berkshire home - something he is now suing the BBC over.
Former bandmate Tony Rivers wrote on Facebook: "It has been absolutely depressing for Sir Cliff, two years of hell, with the totally unsubstantiated accusations he's had to live with, other problems and just when the BBC/Police stuff was dropped, he has lost his close family member Donna (his sister) who passed away a day or so ago.
"A change of luck for the future Cliff, [I am] completely with you."
