He started work at the UK government Inland Revenue in 1931. In 1934, he moved to the Treasury. He was involved in financing UK universities, at the time when the University Grants Committee received its funding directly from the Treasury.
In 1947, he worked for a year within the Control Commission for Germany in London. In 1949 he was made a Companion of The Most Honourable Order of the Bath (CB). He then continued at the Treasury until 1956 when he was appointed Permanent Under-Secretary at the War Office. He was appointed a Knight Commander of the Order of the Bath (KCB) in 1957. He was Permanent Secretary at the Ministry of Defence (1960–61).
In the 1960s and 70s, he worked in business. He was the Chairman of International Computers and Tabulators (1961–65), a Director of National Westminster Bank (1961–79), and a Director of Glaxo Holdings (1961–79). During his time at ICT, he was President of the British Computer Society (1963–65). In 1966 he declared himself a "hater of St Pancras" and thus was opposed to Sir John Betjeman's campaign to save the Sir George Gilbert Scott designed Midland Grand Hotel.
Playfair became a trustee (1967–74) and for two years Chairman of the Board (1972–74) of the National Gallery in London. He was also a member of the governing bodies of Imperial College (1958–83) and University College London.
He married a doctor, Molly (née Rae), in 1941 and had three daughters. He died of cancer in London in 1999.
- Noel Annan , Obituary: Sir Edward Playfair, The Independent, 25 March 1999.
- Robert Armstrong, Playfair, Sir Edward Wilder (1909–1999), Oxford Dictionary of National Biography, September 2004. doi:10.1093/ref:odnb/72106.
- Sir Edward Playfair, thePeerage.com.
- BCS Past Presidents, British Computer Society, UK.
- "Eyesore or gem: St Pancras". BBC. 24 June 2007. Retrieved 2 May 2014.