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At Oxford, Boyle met Robert Hooke, who demonstrated his newly invented air pump. Boyle put it to use in investigating the physical properties of air: in New Experiments Physio-Mechanicall, Touching the Spring of the Air and Its Effects (1660) he described the role of air in respiration, combustion, and sound transmission. In 1661 he reported to the Royal Society his discovery that the volume of a gas is inversely proportional to the pressure, a principle now known as Boyle's Law.
In the same year Boyle turned his attention on the basis of matter, challenging both the Aristotelian (and alchemical) principle of the four elements and the three principles (first stated by Paracelsus and later elaborated as Phlogiston theory). He proposed instead an early version of atomic theory, which he spelled out in The Sceptical Chymist (1661).
Boyle was a founding member of the Royal Society, of which he was offered the presidency in 1680 (he declined).
In The Christian Virtuoso (1690), Boyle likened the universe to a piece of machinery set in motion by God, and argued that studying the principles of its operation was a religious duty. Still, he was not a strict mechanist with respect to behavior: he believed in an incorporeal soul that did not follow strict physical laws.