The London Institute for Mathematical Sciences was founded in 2011 by physicists and mathematicians who wanted to spend more of their time on scientific research. The Institute was not endowed early on by a generous benefactor; rather, it grew organically by winning grants, encouraging donations, and hiring new Fellows and postdocs. The Institute is a registered charity: its main activity is making fundamental scientific discoveries and disseminating those discoveries to the public via scientific journals.

The London Institute is entirely research focused and does not award degrees. It is modelled on similar private research centres like the Institute for Advanced Study (U.S.), the Perimiter Institute for Theoretical Physics (Canada), the Curie Institute (France) and the Santa Fe Institute (U.S.).