He was a son of the 1st Baron Llangattock. He was educated at Eton College and Trinity College, Cambridge, and from his youth was interested in engines. He teamed up with Frederick Henry Royce to found the manufacturing company in 1906, Royce providing the technical expertise to go with Rolls's financial backing and business acumen.
Rolls was also a pioneer aviator, and the first man to make a non-stop double crossing of the English Channel by plane. In the same year, 1910, he was killed in an air crash. He was the first Englishman to be killed in an aeronautical accident.