The 75-year-old was born in Newcastle-upon-Tyne and had been living on the Black Isle, near Inverness.
He spent much of the 1960s working in pop art in New York and was a close friend of artists Andy Warhol and Roy Lichtenstein.
Laing's most famous works included images of actresses Brigitte Bardot and Anna Karina.
In October this year, he showcased a series of paintings and drawings of Winehouse in London.
Laing was also a sculptor and created a statue of Sherlock Holmes that stands in Edinburgh and also the Exiles, a statue at Helmsdale that recalls the Highland Clearances in Scotland.
Four Rugby Players at Twickenham Stadium, Ten Dragons at London's Bank Underground Station and The Glass Virgins at Standard Life's building in Edinburgh are among his other sculptures.
It was understood Laing had been battling cancer.
The artist's son Farquhar said his father had been a truly talented man.
Speaking at his family home at Kinkell Castle on the Black Isle, he said his father painted, sculpted, drew and rebuilt cars, castles and motorcycles, but added that his outstanding talent was being a great father.
Laing served with the Royal Northumberland Fusiliers following studies at the Royal Military Academy, Sandhurst.
After leaving the Army, he studied at St Martin's School of Art in London and went on live in the US from 1964 until 1969.
He settled in the Scottish Highlands and rebuilt 16th Century Kinkell Castle.
Artist Gerald Laing whose latest work included pop art featuring the late singer Amy Winehouse has died.