Bloembergen met Huberta Deliana Brink (Deli) in 1948 while on vacation with his university's Physics Club. She was able to travel with him to the United States in 1949 on a student hospitality exchange program; he proposed to her when they arrived in the States, and were married by 1950 on return to Amsterdam. They were both naturalized as citizens of the United States in 1958. They had three children.
Bloembergen died on September 5, 2017, at an assisted living facility in his hometown Tucson, Arizona, of cardiorespiratory failure, at the age of 97.