The Society had its origins in the 1844 ordinance passed by the Second Municipality Council, "Providing for the establishment of a Lyceum and Library by the Scholars of the Public Schools of Municipality No. Two." That law created a "Lyceum and Library" whose cost was to be defrayed by voluntary contributions of the students (not to exceed twenty-five cents per month or $3.00 annually). Upon making a total contribution of $9.00 the student became a life member of the Society. Other individuals could become subscribers to the library at terms set by the board of directors, which was identical to the directors of the public schools in the municipality. Certain public officials were ex-officio members and public school teachers were honorary members. Once $5,000 was collected and paid into the Treasury the Municipality would provide rooms for the library, and when $15,000 had been paid in, a lot and building would be make available to the institution. In addition to payments by the students, donations were also accepted from interested individuals.

The library opened on March 10, 1846 with 3,400 books in its collection; by 1858 it held over 10,000 volumes. Originally located in temporary quarters, the Lyceum Library moved into the new municipality hall (now Gallier Hall) when its rooms in that building were ready for occupancy.

Following consolidation of the city in 1852 the library apparently continued operating in what by then was the City Hall. It was known as the Lyceum and Library Society, First District. Similar facilities were to be established in the other three municipal districts, but none of the others appears to have developed to the extent of the First District's. In 1859, ordinance #4439 gave the Society's directors the power to open up membership to all white youths in the city and to such other contributors as they saw fit to include. The directors could also issue honorary memberships as they deemed appropriate.

During the Civil War occupation, probably in 1863, ordinance #6140 provided for the consolidation of the district libraries into a single institution located in City Hall and known as the "public library of the city of New Orleans." The books of the First District Lyceum apparently formed the core of the new collection, and the name "Lyceum and Library Society" remained in popular use. The 1863 ordinance, along with #1276 in 1869 (which provided that the Lyceum's directors would be appointed by the Mayor), signalled an evident end to the library's association with the public schools.

The Lyceum and Library Society continued to function as a separate entity until 1896 when the city merged it with the Fisk Library to form the New Orleans Public Library.