Rafaelian’s father opened a jewelry factory in 1966, in which Rafaelian and her sister worked. Over time she helped her father design pieces and produced original designs herself for her father’s jewelry manufacturing company Cinerama. She attended Prout Memorial High School for Girls (later known as The Prout School). She attended the University of Rhode Island between 1987 and 1989, and then she transferred to and graduated from the American College in Los Angeles. In 1994 she joined her father’s business, and eventually began to work on her own line. In 2002 Rafaelian became co-owner of Cinerama with her sister. Rafaelian’s designs became the main seller for the company, and in 2016 Alex and Ani bought the manufacturing facility for an undisclosed sum.

In 2004 Rafaelian founded Alex and Ani, a jewelry line named after her two eldest daughters. The brand started with five cocktail rings and expanded into a full line of jewelry anchored by its patented expandable wire bangle.

Rafaelian has been interviewed by newspapers regarding current events, including the New York Daily News. Rafaelian received the 2012 Rhode Island Small Businessperson of the Year award from the Small Business Administration for her work with Alex and Ani, and also the Ernst & Young Entrepreneur of Year in the products category for New England. Her firm’s revenue grew from $5 million in 2010 to over $500 million in 2016 and the company’s Charity By Design initiative, where 20% of sales go to charity, makes up 20% of sales.

Rafaelian owns a cafe franchise called Teas and Javas; some of its cafes are attached to Alex and Ani stores, and some are independent. She is also the owner of the Rhode Island winery Carolyn’s Sakonnet Vineyard, purchased in 2012 which features wine making, dining area and locally sourced foods. Since taking over, the vinyard has won a number of awards in international competition.

Rafaelian was listed 22nd in Forbes America’s Richest Self-Made Women in 2016, with net worth estimated at $700 million in June 2016. In May 2017, she was recognized by the David Lynch Foundation for her humanitarian efforts. In June 2018, Rafaelian was estimated to be worth $1 billion, and 18th on the Forbes list of America’s richest self-made women, owning 80% of Alex and Ani. By June 2019 her net worth had dropped to an estimated $520 million.