Zhou started acting in 1935, but she achieved stardom in 1937 in Street Angel (街角天使 jiējiǎo tiānshǐ) , when director Yuan Muzhi cast her as one of the leads as a singing girl.

"Golden Voice" was Zhou's nickname to commend her singing talents after a singing competition in Shanghai, where she came in second. Zhou rapidly became the most famous and marketable popular singer in the gramophone era up to her death, singing many famous tunes from her own movies. Her frail but eminently musical voice captured the hearts of millions of Chinese of her time.

After introducing "Nightlife In Shanghai", Zhou returned to Shanghai. She spent the next few years in and out of mental institutions owing to frequent breakdowns. Through the years, Zhou led a complicated and unhappy life marked by her failed marriages, illegitimate children and suicide attempts.

Having made a total of 43 movies. Her favourite film was always Street Angel. This contained two theme songs: "Four Seasons Song" (四季歌 sìjì gē) and "The Wandering Songstress" (天涯歌女 tiānyá gēnǚ) which enjoyed long-lasting popularity.

Her recordings can be found through CRC Jianian, a joint-venture between the Chinese government and American publishers.