Phi Beta Kappa, the oldest and most prestigious undergraduate honors society in the United States, recognizes achievement in the liberal arts. The society was founded on December 5, 1776, at the College of William and Mary in Williamsburg, Virginia. The beginnings of Phi Beta Kappa at Connecticut College occurred in 1925 with the formation of the New London Phi Beta Kappa Association. Spearheaded by the College's second president, Benjamin Marshall, the association was open to PBK members who were on the College faculty or who resided in New London.

The next milestone occurred three years later when, on May 7, 1928, the faculty voted to establish the Winthrop Scholar Program to recognize students who attained high grades throughout their coursework. This program (named for John Winthrop the Younger, who founded New London and served as governor of Connecticut) fulfilled a long-standing desire to make more marked recognition of high scholarship at Connecticut College. On June 9th of that same year, the faculty voted to make this distinction retroactive for those who had previously received their degree from the College.

Under the leadership of President Katherine Blunt, Connecticut College made application for a PBK chapter to the Council of the United Chapters of Phi Beta Kappa. In September 1934, at their 18th triennial meeting, the Council granted a charter to the College for the establishment of a chapter. The Delta of Connecticut chapter was installed at Connecticut College on February 13, 1935. At that time, the faculty voted to retain the designation of Winthrop Scholar as its highest honor, reserved for students elected to Phi Beta Kappa in the fall term of their senior year.

In the years since, new members have been inducted each year. The Delta of Connecticut chapter has brought guest speakers to campus through the Phi Beta Kappa Visiting Scholars program, and sponsors a scholarship to support alumni of Connecticut College who are attending graduate school. Representatives of the chapter have also attended Triennial Council meetings at the national level. In 2024 the Winthrop Scholars distinction was renamed to Susanne K. Langer Scholars, to honor the former Professor of Philosophy.