The preponderance of Serbian materials in the Library of Congress is held in the general collections. Consisting of thousands of books, journals, and pamphlets, the materials cover all possible subjects with the exception of clinical medicine and technical agriculture, which are collected by the National Library of Medicine and the National Agriculture Library. Materials held in the general collections are findable by searching the Library of Congress Online Catalog.

The largest subject is language and literature covering 33% of the Serbian book collection. Represented are collected works and individual titles for all of the major Serbian authors and poets from all eras, as well as many works of minor writers. There are reprints of old Slavic manuscripts and the works of scholars and writers who led the transition from religious to secular writing and from using Church Slavic to native Serbian such as Vuk Karadžić and Dositej Obradović. The Library has most of the important dictionaries for Serbian such as the dictionaries from Vuk Karadžić, Đuro Daničić, and Grigorije Lazić, plus the latest Matica srpska dictionary, as well as many smaller, specialized works and historical, etymological, and bilingual dictionaries. Grammars, language textbooks, and linguistic studies are collected extensively.

The history and politics of Serbia, Yugoslavia, and the Balkan peoples is a particular strength, comprising almost 23% of the Serbian book collection. Books on all aspects of Serbian history and politics are collected, including the works of all major publishers and contemporary scholars such as the Herder Prize winner Andrej Mitrović - Srbija u Prvom svetskom ratu [Serbia in the First World War]. Holdings for the communist and post-communist eras are extensive containing the collected works and speeches of major political figures such as Josip Broz Tito, Slobodan Milošević, and Zoran Đinđić. All of the major historical journals are held including Istorija 20. veka: časopis Instituta za savremenu istoriju [History of the 20th century: the journal of the Institute of Contemporary History], Godišnjak za društvenu istoriju [Annual of social history], and Tokovi istorije: časopis Instituta za noviju istoriju Srbije [Currents of history: journal of the Institute for Recent History of Serbia]. Books about World War II are prevalent, but titles published in Serbia during the war are less so. Religious studies amount to about 4% of the Serbian collection, which is significant in comparison with similar holdings of other North American libraries. Weak spots in the Serbian holdings include military and naval science and agriculture, with only several hundred titles on each topic in the collection.

Although the majority of Serbian materials in the Library of Congress are published in Beograd, titles from other cities comprise approximately 24% of the collection rendering regional publications a relative strong point. Novi Sad is the largest regional city of publication in the collection, making up 9% of the collection with over 4,800 titles, followed by Niš with over 900 titles. Rounding out the collection are books from the diaspora, which emanate from all over the world with the three largest diaspora sources in the collection being the U.S., Romania, and Germany. Overall, the collection is strongest for the post World War II period. Also of note are the thousands of books touching on the subject of Serbia or Yugoslavia in English and other West European languages, as well as languages of the other countries in Southeast Europe.

The collection is rich in government publications, both historical and current. There are nearly complete holdings of the records of parliament up until the post-Yugoslav era, Serbian and Yugoslav census data from various historical periods, many publications of the Narodna banka Jugoslavije and the National Bank of Serbia, and other Serbian statistical materials, ranging from the various iterations of the main statistical almanac, Statistički godišnjak Srbije [Statistical annual of Serbia], to specialty compilations on economics, culture, and agriculture.

Recognizing that historians, genealogists, and business researchers frequently need to consult directories, the Library of Congress maintains a collection of international telephone directories. Business and specialized directories from Serbia are cataloged and may be identified using the Library of Congress Online Catalog. Uncataloged telephone directories from Serbia may be identified using the guide Serbia: Address and Telephone Directories. The uncataloged collection contains almost 100 volumes from 1936 to 2008. For uncataloged items in the general collections, a researcher must request the items by completing a call slip in the Main Reading Room or asking in person for help in the European Reading Room. Selected directories also have been digitized and are freely available on the Library of Congress website. Other directories from a microfilm collection of Yugoslav phone books also have been digitized and are available onsite only in the Library of Congress digital repository called Stacks.