The College Library was founded in the college in 1863, just a year after Miller arrived. This facility was upgraded as a Consulting Library in 1869, containing dictionaries, atlases, commentaries and books of Reference of every branch of knowledge. This was open for the students of the college for one hour before the commencement and two hours after the college was closed. In 1870 about 200 students had free access to the General Library, and over a thousand books were borrowed in a year. It was so efficiently managed that not a single volume was found missing. In 1871, Mrs Margaret Gunn of Latheron, Scotland endowed the Library with a sum of 1000 Pounds in memory of her husband Donald Gunn who died in 1869. The interest of this sum was made available for the maintenance of the Library. The Hunter Commission on Education in 1882 gave a high commendation to the richness of the Library, along with that of the Presidency College.

The system of Class Libraries was introduced in 1886, pertaining to the departments of Mathematics, Physical Science, Natural Science, Mental and Moral Science. There were more than 100 volumes in each of these class libraries. Miller himself had a fine library for himself which he subsequently donated to the college. A consulting Library was also started with a gift of books from Messrs Blackie & Co., Special class libraries were also started, along with an exclusive one for MA students. Interestingly, Professors acted as Librarians in turn. Professor Laidlaw as the Librarian in 1892 printed the catalogue; Professor Kellett in the following year procured several volumes as gifts from prestigious publication houses and individuals, which included the Cambridge University Press, the Clarendon Press; Professor Max Muller himself donated a splendid new edition of his commentary of Rg. Veda.

A Reading room where more magazines and periodicals were placed, was opened in 1896. For the first time a full-time official—the Assistant Librarian—P.Rama Aiyar was appointed in 1904. The Library for the Institution’s school was bifurcated with 800 volumes in the year 1909, as until then the Library was also used by the school students of higher classes. After the introduction of the Honours courses in 1911, there were many significant changes, one of which was opening the Library during night times between 7 and 9 pm. The College Hall was fitted with electric lights and fans for this purpose, even as most students of the college did not enjoy such a luxury. The Library facilities gradually increased thereafter, and by 1920 there were more than 7200 volumes stacked in the General Library.

When the college was relocated to Tambaram campus, the first building to be inaugurated by the Governor Lord Erskine, on January 30, 1937, was the Miller Memorial Library. The very fact that it was named after the illustrious Principal kindled generous response in scores of alumni to contribute to the building fund. The next 50 years it was located in the present Examination Hall, with its first floor being used as a Reference section.

The Miller Memorial Library celebrated its Centenary in December 1963, with S.R. Ranganathan, an alumnus and the father of Library movement in India, participating as chief guest.G.S.Theophilus served as the first Librarian in Tambaram (1937-55), followed by Baktamitran, Mrs.Kasthuri Guruswami, and V.C.S, Rajappa, Dr.P.Yesudoss (2012-Till date)