Nasrollah Afjei was born in 1933 in Tehran. From a young age, he exhibited a strong interest and talent in calligraphy, painting, and music. At 15, he began his career in an atelier and, after a year, opened his own studio with a friend.

Upon completing his schooling, Afjei attended the Miniature Advertising Center, which he considered an art academy. Owned by Rassam Arabzadeh, this center allowed him to learn calligraphy from masters such as Kimia Ghalam Zanjani and Ali Akbar Kaveh. After finishing his military service in 1957, Afjei, along with friends Ali Akbar Sadeghi, Ali Reza, and Mahmoud Basiri, founded "Atelier Seven" on Baharestan Street in Tehran. This studio became a focal point for their artistic endeavors and attracted prominent artists including Morteza Momayez, Parviz Kalantari, and Abbas Kiarostami.

Afjei's work was first exhibited internationally in 1974 at the International Painting Exhibition in Switzerland. Over the years, his calligraphic paintings have been showcased in various countries, including France, England, the United States, and Germany. In 1993, he was awarded the first-class artistic award by the Ministry of Guidance and Islamic Culture. Additionally, Afjei has been actively involved in art education, teaching at the University of Tehran, Al-Zahra University, and Sooreh University.

During the 1960s and 70s, Afjei experimented with blending calligraphy and modern painting, influenced by neo-traditionalist art movements, particularly the Saqqa-khaneh movement. He presented these works in an exhibition titled "Calligraphic-Painting" at the Seyhoon Gallery. Afjei coined the term "Calligraphic-Painting," which later came to describe works combining painting and calligraphy.

In his calligraphic paintings, Afjei not only explored the potential of calligraphy but also integrated elements of the Iranian-Islamic tradition of calligraphy and page layout. Art critic Ruyin Pakbaz observed that "Afjei's expertise in various traditional calligraphy methods has diversified his calligraphic paintings. In the 1970s, Afjei created Op Art-inspired works using the Kufic-Bannai script and crafted deliberate compositions with Thuluth script features. Since the early 1970s, he has developed a more personalized style based on the Siyah mashq tradition, creating intricate combinations with hidden Nasta'liq intertwined letters."