He is currently on faculty at Florida State University, which he joined in 2004, and prior to that he spent a large part of his working career at the University of Sussex, where he holds an emeritus professorship.
As a child, he became fascinated by a Meccano set. Kroto credits Meccano — amongst other things — with developing skills useful in scientific research . He was raised Jewish, but the religion never made any sense to him.
Among other things such as making the first phosphaalkenes (compounds with carbon phosphorus double bonds), his doctoral studies included some unpublished research on carbon suboxide, O=C=C=C=O, and this led to a general interest in molecules containing chains of carbon atoms with numerous multiple bonds. He started his work with an interest in organic chemistry, but when he learned about spectroscopy it inclined him to quantum chemistry.
After postdoctoral research at the National Research Council in Canada and Bell Laboratories in the USA he began teaching and research at the University of Sussex in England in 1967. He became a full professor in 1985, and a Royal Society Research Professor from 1991 – 2001.
Trying to explain them led to the discovery of the C60 molecule. (See buckminsterfullerene.) He heard of laser spectroscopy work being done by Richard Smalley and Robert Curl at Rice University in Texas. He suggested that they should use the Rice apparatus to simulate the carbon chemistry that occurs in the atmosphere of a carbon star.
The experiment carried out in September 1985 not only proved that carbon stars could produce the chains but revealed an amazing, serendipitous result - the existence of the C60 species. The three scientists carried out the work with graduate students Jim Heath (now a full Professor at Caltech), Sean O'Brien (now at Texas Instruments), and Yuan Liu (now at Oak Ridge). The Nobel Prize in Chemistry was shared by Curl, Kroto and Smalley in 1996.
In 1995 he jointly set up the Vega Science Trust a UK educational charity (see www.vega.org.uk) to create high quality science films including lectures, interviews with Nobel Laureates, discussion programmes, careers and teaching resources for TV and Internet Broadcast. Vega has produced some 100 plus programmes of which 50 have been broadcast on BBC TV in late-night slots. Additionally, all programmes stream for free from the Vega website which acts as a TV science channel. Viewing figures on terrestrial TV vary from 300,000 to 700,000. The website which is accessed by over 165 countries is designed by Harry Kroto and shows his other main interest - graphic design.
Kroto currently researches at Florida State University where it is widely known that he is lobbying Florida State University President T.K. Wetherell to make Bobby Bowden "dissappear" or else he will leave the University and take his grant money with him. Citing their lack of chemistry and saying "this university is not big enough for the both of us.. He presently carries out research in Nanoscience and Nanotechnology.
He attended and was a speaker at the Beyond Belief symposia in 2006 and 2007.
In 1963 he married Margaret Henrietta Hunter, also a student at the University.