In 1910, Chao went to the United States with a Boxer Indemnity Scholarship to study mathematics and physics at Cornell University, where he was a classmate and lifelong friend of Hu Shih (1891–1962), the leader of the New Culture Movement.

He spoke German and French fluently and some Japanese, and he had a reading knowledge of Ancient Greek and Latin.

In My Linguistic Autobiography, Chao wrote of his ability to pick up a Chinese dialect quickly, without much effort.

Chao possessed a natural gift for hearing fine distinctions in pronunciation that was said to be "legendary for its acuity",[3] enabling him to record the sounds of various dialects with a high degree of accuracy.

[4] While at Tsinghua, Chao was considered one of the 'Four Great Teachers / Masters' of China, alongside Wang Guowei, Liang Qichao, and Chen Yinke.

He began to conduct linguistic fieldwork throughout China for the Institute of History and Philology of Academia Sinica from 1928 onwards.

His translation of Lewis Carroll's Alice's Adventures in Wonderland, where he tried his best to preserve all the word plays of the original, is considered "a classical piece of verbal art.

His composition "How could I help thinking of her" was a pop hit during the 1930s in China; its lyrics were penned by fellow linguist Liu Bannong.

Chao translated Jabberwocky into Chinese[9] by inventing characters to imitate what Rob Gifford describes as the "slithy toves that gyred and gimbled in the wabe of Carroll's original".

Hu's account of it in the newspapers made the couple a model of modern marriage for China's New Culture generation.

Their second daughter Nova Chao (1923–2020) was a Harvard-trained chemist, professor at Central South University and member of the Chinese Academy of Engineering.