The work undertaken by the Centre for Entrepreneurs focuses on obstructions to entrepreneurship in the UK, and geographical areas where more regeneration and entrepreneurial thinking are required.

The Centre offers various entrepreneurial development programmes, builds entrepreneurial communities and engages policymakers in key conversations around innovation. Research reports drive the Centre’s work and consider entrepreneurship's necessity, the barriers to opportunity, and how to unlock the potential for neglected and marginalised communities and individuals.

The Centre operates as a think tank for entrepreneurship by producing a series of research reports on topics such as prison entrepreneurship, the importance of immigrant entrepreneurship and how entrepreneurship can rejuvenate British seaside towns. Another example of their work is the Refugee Entrepreneurship Pilot Programme, jointly funded by the National Lottery and the Home Office. The Centre has also worked with, led and supported Start Up Britain.

In 2017, the Centre joined forces with New Entrepreneurs Foundation to become the UK's entrepreneurial powerhouse, which was made possible through the support and dedication of Letter One. This is an excellent example of how Legatum originates, incubates and then scales and releases its ideas into the world.

Today, the Centre runs the NEF+ Fast Track programme, a 12-month entrepreneurship programme providing mentorship, training, networking opportunities and real-world business experience to each of its participants.