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It's a three way tie between:
Leaded Gas
Aerosols
Nuclear bombs
Interesting fact, the same man, Thomas Midgely Jr, invented both tetraethyl-lead as a fuel additive and CFCs, almost killing everyone on earth twice over.
Karma got him in the end after he got tangled in one of his contraptions after he became bedridden with polio and died of strangulation.
https://en.wikipedia.org/wiki/Thomas_Midgley_Jr.
I first read of him in Bill Bryson's A Short History of Nearly Everything (fantastic book). It really shows how awful this man was.
I also love this quote from the wiki article on his legacy -
He "had more adverse impact on the atmosphere than any other single organism in Earth's history".