In 1966, Taiwo Ajai-Lycett unexpectedly began her acting journey in a play's rehearsal hall. She performed in a comedy called "The Lion and the Jewel" at the Royal Court Theatre in London. Her impressive performance led to more opportunities, and she decided to pursue acting seriously. She honed her skills at the Guildhall School of Music and Drama. In 1972, she left her corporate job and joined the Traverse Theatre Group for a festival in Edinburgh. From there, she appeared in various TV shows and stage productions. Notable highlights include roles in plays like "Life Everlasting" and "The National Health" in London. In 1976, she starred in "Parcel Post" at the Royal Court Theatre. She was also involved in directing with the Black Theatre Workshop in London, along with Louis Mahoney and Mike Phillips. Returning to Nigeria in 1971, Ajai-Lycett became part of notable Nigerian films, including the popular soap opera "Tinsel." She also featured in the Nigerian movie "Oloibiri," a 2016 action thriller that sheds light on the exploitation of newly discovered oil in Oloibiri town by government agencies and oil companies.