Nasrollah Afjei was born in 1933 in Tehran. He was interested in calligraphy, painting and music from childhood and showed his talent in his childhood. He started his career at the age of 15 in an atelier and after a year launched his own one with one of his friends.

After graduating from school, Afjei went to the "Miniature Advertising Center". He refers to the center, which belonged to Rassam Arabzadeh, as an art academy. He got the opportunity to accompany and learn calligraphy from masters such as Kimia Ghalam Zanjani and Ali Akbar Kaveh there. After the end of his military service in 1957, together with his friends Ali Akbar Sadeghi, Ali Reza and Mahmoud Basiri, he set up "Atelier Seven" on Baharestan Street. This studio became the focal point for him and his friends' ongoing activities. Great artists such as Morteza Momayez, Parviz Kalantari and Abbas Kiarostami came to this studio. 

The first overseas appearance of his works took place in 1974 at the International Painting Exhibition in Switzerland. His calligraphic paintings have been exhibited in various countries such as France, England, America and Germany in recent years. In 1993, Afjei received the first-class artistic award from the Ministry of Guidance and Islamic Culture. He has also been active in art education for many years; Teaching at the University of Tehran, Al-Zahra University, Soureh University, are some of his educational activities. Nasrollah Afjei's first appearance in the auctions goes back to June 2008 at the Christie's Auction House. 

Afjei used calligraphy in the form of modern painting in experimental works in the period of 60s to 70s under the influence of traditionalist art movements, specifically the Sagha Khaneh movement and exhibited the resulting artworks in an exhibition called “calligraphic painting” at the Seyhoun Gallery. "Calligraphic painting" was an innovative title by Afjei which later applied to works that combined painting and calligraphy. In addition to exploiting the potential of calligraphy, Afjei has used some features of the Iranian-Islamic tradition of calligraphy and page layout in combining and arranging the elements of his calligraphic paintings. Ruyin Pakbaz writes about him: "Afjei's expertise in various methods of traditional calligraphy has diversified his calligraphic paintings. In the 1970s, he created Op Art-inspired works using Kufic-Bannai script, or exploited Thuluth script features in deliberate compositions. "Since the early 1970s, he has developed a more personalized style based on the Siyah mashq tradition, creating extensive combinations with hidden Nasta'liq intertwined letters."