Peggy Angus was a painter, first and foremost, but she became best known for her crafts, designing tiles and creating hand-printed wallpaper from carved linoleum blocks. Her paintings of John Piper and the family of Ramsay MacDonald hang in the National Portrait Gallery in London.

She rented an unimproved shepherd’s cottage (Furlongs, near Beddingham) at the foot of the South Downs, and made that a home to which a circle of artists of gathered. These included Eric Ravilious and John Piper. Eric Ravilious considered that his time at Furlongs "…altered my whole outlook and way of painting, I think because the colour of the landscape was so lovely and the design so beautifully obvious … that I simply had to abandon my tinted drawings".

Peggy Angus taught art for many years at the North London Collegiate School for Girls. She galvanised the girls to improve their environment, daubing the walls of the school buildings with repeat patterns of bright colours.

The architect F.R.S. Yorke saw the potential of the repeat patterns as tiles to bring life to the interiors of modern buildings. Carter & Co began to produce her designs commercially. She tested her designs on demonstration lengths of lining paper, which became the inspiration for rolls of wallpaper of repeating designs, in which no two prints were ever exactly the same, used by Cole and Sandersons and fabrics.
Peggy Angus etched marble decoration for glass cladding. She invented Anguside, used in the building of Gatwick Airport.