In 1901, postmaster Walter Chapman stabbed to death his wife Emily and was found guilty but insane and committed to Broadmoor Hospital.

The National School was founded in 1871 on land provided by the architect Edward I'Anson, who had moved to the village ten years earlier.

His descendants maintained a close connection to the area (his son made funds available for the construction of the church) and many of these are buried and memorialised in its churchyard.

There is a long history of amateur drama in the village, beginning before World War 1 and continuing to the present day.

Ludshott Common, one mile to the west, is an area of heathland and woodland and part of the East Hampshire Area of Outstanding Natural Beauty;[13] one mile to the east is Hindhead and the Devil's Punch Bowl, a site of special scientific interest, and to the north is the Golden Valley, a densely wooded valley between the B3002 and A287 roads.

[18] From 1898 to 1900 Flora Thompson,[19] author of Lark Rise to Candleford, was assistant postmistress in Grayshott and lived in The Avenue.

Among her customers were Arthur Conan Doyle, who lived at Undershaw (which became the Undershaw Hotel, now a school for pupils with special needs) next to Hindhead crossroads, and George Bernard Shaw, who lived at Blen Cathra, Boundary Road, now St Edmund's School, Hindhead.

Dame Agnes Weston (1840–1918), philanthropist and founder of the Royal Naval Sailors' Rests, lived in Crossways Road for a number of years.

This building, known as Grayshott Hall, is on the site of a small farm which Alfred Tennyson and his family rented in 1867 while he had Aldworth built nearby in Haslemere.

Grayshott is the birthplace of actor Colin Firth, best known for his appearances in films such as Bridget Jones's Diary, Mamma Mia!, A Single Man and The King's Speech.