Monroe is the Gilhuly Family Presidential Distinguished Professor of Electrical and Computer Engineering and Physics at Duke University[4] and was College Park Professor of Physics at the University of Maryland and Fellow of the Joint Quantum Institute and Joint Center for Quantum Computer Science until 2020 when he moved to Duke.

He is also co-founder of IonQ, Inc. After receiving his undergraduate degree from MIT in 1987, Monroe joined Carl Wieman's research group at the University of Colorado in the early days of laser cooling and trapping of atoms.

With Wieman and postdoctoral researcher Eric Cornell, Monroe contributed to the path for cooling a gas of atoms to the Bose-Einstein condensation phase transition.

In 2000, Monroe initiated a research group at the University of Michigan, Ann Arbor, where he showed how qubit memories could be linked to single photons for quantum networking.

In 2021, Monroe became the Gilhuly Family Presidential Distinguished Professor at Duke University, in the Departments of Physics and Electrical and Computer Engineering.