Many different collections constitute the treasury and the book depository of the NPLG.

Among them, the private collection of Michael Voronstov, Governor-General of the Caucasus and donated to the Public Library of Tbilisi; 3 000 items from the private collection of Evgeni Veidenbaum, the famous researcher of the Caucasus; collection of of the well-known historian Simon Esadze, Director of the Public Library; and collection of Professor Giorgi Gechtman, the first Director of the Public Library, should be mentioned.

The collection of the Society of Propagation of Literacy among the Georgians, is the most valuable part of the library - where the private collections of Georgian princes and nobility, the Ruler of Samegrelo David Dadiani, private collections of famous public figures of the 19th century - David Chubinashvili, Rafiel Eristavi, Jacob Gogebashvili, Peter Umikashvili, historian Dimitri Bakradze are united. One of the most remarkable collection of this field is the Ilia Chavchavadze’s private library.

The collection became the basis of the Archive Funds of Georgian Printed Items, founded in 1937, which in year 1999 developed into separate scientific department. Valuable purchase for the library was the collection of books of prosperous merchant of the XIX century, Basilius and Michael Tamamshevs. Most of the books were concerning art and world history topics. Niko Nikoladze’s archive and a part of his library, which were donated in several parts in 1920, 1941 and 1960 years.

A complete collection of the first printed Georgian books is stored in the Rare Books Department. There are united rare publications such as the first Georgian books – 'Georgian-Italian Dictionary' printed in Rome by Catholic missionary press in 1629, 'Davitni' (David’s Psalms) printed by King Archil II in Moscow in 1705, the most rare 'Davitni' printed in the press of King Vakhtang VI in 1709, and the famous 'The Knight in Panther’s Skin' by Shota Rustaveli printed in 1712 . The Library has in its possession complete collection of printed publications existing in Georgia, printed in the first Georgian press established by King Vakhtang VI. 'Verdict of Jerusalem' of IX century and 'Gospel' of XIII century are among the precious manuscripts collection of the Library. 

Entire collections of books of the NPLG by language consist of 532 523 (14,7%) Georgian and 3 091 469 (85.3%) foreign books, among them 152 419 (4.3%) European,  2 876 300 (79.3%) Russian and 62,750 (1.7%) in other languages.

In the collection of periodical publications are kept the richest collections of printed periodicals in Georgian, Russian, Armenian, Azeri, Abkhazian, Ossetian and other languages, the press of European countries and scientific periodicals in English, French, Italian and German languages; the press and scientific periodicals of the USA.  Annual sets of central newspapers of former Soviet Union Republics printed in 1921-89 years.

Among the collections is the first Georgian newspaper printed in 1819 - 'Sakartvelos Gazeti', complete sets of newspapers 'Iveria', 'Droeba', 'Tsnobis Purtseli', the press of the repressive years of 1920s, rare periodicals of the first Democratic Republic of Georgia.

The Library has in its possession remarkable collections of printed music and audio-visual publications, cartographic collections, microfilms/microfiches, scripts and archives of documents and materials. 

The compact discs collection is in the process of its formation.