According to a source at the Queen's nearby Sandringham Estate the demands of the role had become too much.
Sadie Rice, 35, has been working at the home in Norfolk for two years, but reportedly refused to spend more time with the family at their home in Kensington Palace.
Sadie Rice, 35, announced her decision to leave after almost two years in the £35,000-per-year ($44,000) job, having previously worked for Norway's Prince Haakon and wife Mette-Marit in the nation's capital, Oslo, where she spent five years.
Ms Rice's departure will be inconvenient at a time when William and Kate have been seeking to expand their household staff.
The woman's responsibilities at Kensington were increasing a lot, and they even asked her to spend more time at the residence.
Like a modern day Cinderella, the Duchess of Cambridge went from being a commoner to a real life princess but now it seems she may have to don an apron once again after her top housekeeper suddenly quit.
Apparently, their main housekeeper has made a decision to quit her job and insiders revealed that there is nothing that "will change her mind" and make her come back.
A Sandringham insider told the Daily Mail the mother-of-two was a "welcome addition", adding: "She is very popular and friendly and George and Charlotte already get on well with her and her kids - she has a boy and a girl".
Before that she was a Buckingham Palace maid and was well liked by the Queen.
Anmer Hall where William and Kate lived while George attended nursery.
Kate and Wills have been hiring more staff to prepare for their move to west London.
Prince Harry's girlfriend, actress Meghan Markle, is also a regular visitor at his two-bedroom cottage in the grounds of Kensington Palace.