The preponderance of Croatian 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. Represented are collected works and individual titles for all of the major Croatian authors and poets from all eras, as well as many works of minor writers. In the collection are several important books on the history of South Slavic languages: Grammatik der illyrischen Sprache (Vienna, 1854) by Andrija Torkvat Brlić; and Ilirska slovnica (Zagreb, 1854) by Vjekoslav Babukić. The Library has most of the important dictionaries for Croatian such as the Academy dictionary Rječnik hrvatskoga ili srpskoga jezika (Zagreb, 1880-1976), Petar Skok's 4-volume etymological dictionary Etimologijski rječnik hrvatskoga ili srpskoga jezika (Zagreb, 1971-74), 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 Croatia and the Balkan peoples is a particular strength of the collection. Books on all aspects of Croatian history and politics are collected, including the works of all major publishers and scholars from all eras, but books from the communist era are particularly extensive. Examples of historical titles include Znameniti i zasluzni Hrvati te pomena vrijedna lica u hrvatskoj povijesti od 925-1925 (Zagreb, 1925), Generalno učilište Dominikanskoga reda u Zadru ili "Universitas Jadertina" 1396-1807 (Zadar, 1996), and the many works of Ferdo Šišić (1869-1940). Croatians living outside their state made a significant contribution in publishing the memoirs of prominent participants in Croatia's recent history and describing their history from various perspectives. Here notable titles are Ivo Korsky, Hrvatski nacionalizam (a history of Croatia from 1918 to 1945) and Vjekoslav Vrančić, Branili smo drzavu, as well as the memoirs of the leader of the post-Yugoslav country of Croatia, Franjo Tudjman's Bespuca povijesne zbiljnosti (1989). All of the major historical journals are held in print and/or digital formats such as Časopis za suvremenu povijest [Journal of Contemporary History] from Zagreb, Kulturna baština [Cultural Heritage] from Split, and Povijesni prilozi [Historical Contributions], also from Zagreb.

Although the majority of Croatian materials in the Library of Congress are published in Zagreb, titles from other cities comprise approximately 25% of the collection making regional publications a relative strong point. Military history is a weak spot in the Croatian collection, with only several hundred titles held. Books about World War II are prevalent, but titles published in Croatia during the war are less so. 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 Croatia 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, Croatian census data from various historical periods, publications of the Croatian National Bank, and other Croatian statistical materials, ranging from the various iterations of the main statistical almanac, Statistički ljetopis [Statistical annual], 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 Croatia are cataloged and may be identified using the Library of Congress Online Catalog. Uncataloged telephone directories from Croatia may be identified using the guide Croatia: Address and Telephone Directories. The uncataloged collection contains over 100 volumes from 1948 to 2015. Also of interest may be some titles listed in the telephone directory guide for Former Yugoslavia. 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.