Olive Muriel Cook was born in Chesterton, a suburb of Cambridge, England, to Arthur Hugh Cook, an assistant at Cambridge University Library, and his wife, Kate Webb Cook. Olive won scholarships to The Perse School and then to Cambridge University, Newnham College. There she read Modern Languages and graduated in 1931. She went to work for Chatto & Windus as a typographer and then moved on to the National Gallery, where she was supervisor of publications under the directorship of Sir Kenneth Clark.
Olive was a self-taught painter and some of her watercolors were acquired for the Recording Britain project during World War II. After the war, she worked as a freelance writer and artist, and wrote country guides, such as Suffolk (1948), part of the Vision of England series, and Cambridgeshire: Aspects of a County (1953). In 1954, she married photographer and architect Edwin Smith and together they wrote and illustrated books and articles on the wonders of English architecture and culture. These included contributions to Leonard Russell's annual Saturday Book (1944 to the 1960s), as well as the English Parish Churches series (1950s), English Cottages and Farmhouses (1954), English Abbeys and Priories (1961), The English House Through Seven Centuries (1968), English Cathedrals (1989), and more. The couple participated in the movement seeking to preserve local traditions, rural skills and crafts.
In 1962, they moved to Saffron Walden, where they renovated an old house and were the driving force behind the idea of creating an Arts Centre. Olive was part of the campaign opposing the building of Stansted Airport, and wrote The Stansted Affair (1967), with a foreword by John Betjeman.