He was a polymath who possessed the second best library in the United States (after that of Thomas Jefferson), and was an indefatigable reader and collector of information at the local national and international level.

He provided a highly sophisticated capsule of current political and cultural news, set in a broad historical context.

He was a strong supporter of public education and frequent tutor and substitute teacher; among the students he taught was Nathaniel Bowditch.

In addition to classic Latin and Greek works, Bentley's collection included books on language, philosophy, the sciences, and early Christianity.

He left the rest of his library to the just-established Allegheny College, founded by fellow Harvard graduate Timothy Alden.

He twice declined Thomas Jefferson's offers of prominent positions, first as chaplain of the United States Congress, and then as first president of the University of Virginia.