"Limitless", based on the feature film, is a fast-paced drama about Brian Finch, who discovers the brain-boosting power of the mysterious drug NZT and is coerced by the FBI into using his extraordinary cognitive abilities to solve complex cases for them. Working closely with Brian in the major case squad in New York City is Agent Rebecca Harris, a formidable investigator with a dark past, and Agent Boyle, a former military officer and Rebecca's confidante. They report to Special Agent in Charge Nasreen "Naz" Pouran, a canny manipulator of the reins of power.

Unbeknownst to the FBI, Brian also has a clandestine relationship with Sen. Edward Mora (Academy Award nominee Bradley Cooper, recurring), a presidential hopeful and regular user of NZT who has plans of his own for his new protege. Fueled now with a steady supply of NZT that enables him to use 100% of his brain capacity, Brian is more effective than all of the FBI agents combined, making him a criminal's worst nightmare and the greatest asset the Bureau has ever possessed.