Buller was the eldest son and heir of Francis Buller, Member of Parliament, of Shillingham near Saltash in Cornwall, by his wife Thomasine Honeywood and was baptised at Saltash on 10 January 1630. His younger brother and eventual heir was John Buller (1632–1716), also a Cornish Member of Parliament.
He was educated at Leyden in 1643 and at Trinity College, Cambridge where he was awarded Bachelor in 1647. He also entered Middle Temple in 1646, received Master of Arts from Oxford in 1649 and was called to the bar in 1652.
In 1660 he was elected Member of Parliament for Saltash in the Convention Parliament and re-elected in 1661 for the Cavalier Parliament remaining until 1679. In1662 he became recorder of Saltash. He was active in parliament on behalf of the tinners of Cornwall.
In 1666 he was tried under the Security Acting for treason on account of indiscrete speech and was fined £30,000.
He lost his own estate and his first wife"s estate was alienated. He received few votes in the election of 1679 and did not stand for parliament again.
Buller died "in a frenzy" at the age of 52.
Cavalier Parliament]
In 1659, Buller was elected Member of Parliament for Cornwall in the Third Protectorate Parliament.
