VNST I is divided into two main groups: official papers or copies of official papers (sections 1-3); and personal papers (section 4). The first three groups include not only Cabinet and Foreign Office papers, which were officially registered, but also some secret official correspondence which did not go through the registry and some semi-official correspondence

VNST II includes personal letters, several from prominent persons, which give a vivid picture of Vansittart's passionate concern about the twin menaces of fascism and communism. There are copies of most of Vansittart's books, plays and poems and many of his articles as well as copies of his broadcasts and some other speeches and correspondence about these.

There is also a small collection of early nineteenth century letters relating to Vansittart's ancestors mainly centered around Nicholas Vansittart who was Chancellor of the Exchequer from 1812 to 1823 and created Baron Bexley in 1823. Somewhat unexpectedly, the collection also contains papers and copies of papers about Lord Kitchener, apparently collected by Sir George Arthur for his book Life of Lord Kitchener.