Volters, born in Riga, studied linguistics in Germany, present-day Estonia, and Ukraine earning his master's degree in 1883.

He established and headed the Central Library (1920–1922), was director of the Kaunas City Museum [lt] (1922–1936), and taught various courses at the Vytautas Magnus University (1922–1934).

Encouraged by professors August Leskien, Karl Brugmann, Aleksander Brückner, Adalbert Bezzenberger, Volters decided to study Baltic languages and culture.

He supported Lithuanian and Latvian students, including Pranas Vaičaitis, Povilas Višinskis, Kazimieras Būga, Antanas Smetona, Rainis, Pēteris Šmits [lv].

He had a reputation as a lenient censor who allowed patriotic and historical plays that glorified episodes from the former Grand Duchy of Lithuania but was stricter on any commentary related to social inequality.

[7] When the city was captured by Poland in the Vilna offensive during the Polish–Soviet War, the library was closed in May 1919 and Volters was invited to Kaunas by President Antanas Smetona.

At the time, Volters believed that both Latvian and Lithuanian were dying languages and cultures that should be studied but not necessarily encouraged or preserved.

In 1887, Volters translated into Lithuanian and prepared for publication Eastern Orthodox liturgy of John Chrysostom in the Cyrillic script.

[5][6] Volters also publicly spoke out against the press ban, including a presentation to the Russian Academy of Sciences in 1887 and an article about the Sietynas case published in Sankt-Peterburgskie Vedomosti in 1897.

[11] In 1883–1884, Volters visited communities of Prussian Lithuanians in East Prussia and collected data about their language and culture focusing on customs and traditions surrounding baptism, weddings, and funerals.

[2] Encouraged by the success, until 1887, he organized annual expeditions to various locations in Lithuania and Latvia (near Vilnius and Švenčionys, Samogitia, Suvalkija, Latgale) to collect ethnographic data.

[12] In 1890, he published a valuable collection of 22 customs from Višķi and 70 Latgalian folk songs with their translation into Russian (Материалы для этнографии латышского племени Витебской губернии).

[1] Volters created and published several questionnaires to collect ethnographic data, including 50-question Program for Indicating the Peculiarities of Lithuanian and Samogitian Dialects (1886), 950-question A Program for Collecting Folk Spiritual Heritage (1892; prepared by students at the Saint Petersburg University under Volters' supervision), and 151-question Ethnographic Data about Latvians (1892; questions on Joninės or St. John's Day; published as in a supplement to Dienas Lapa).

[13] The largest questionnaire primarily dealt with the old Latvian mythology and religion, family and traditional customs, but also had smaller sections on geography and history, anthropology, dwellings, clothing, food and drink, occupations, language and writings.

[12] He collected and published a statistical work on the inhabited localities in the Suwałki Governorate in 1901 (Списки населенных мѣст Сувалкской губерніи).

[14] In expeditions to make the recordings, Volters had several assistants, including Augustinas Voldemaras, Kazimieras Būga, Vincas Krėvė-Mickevičius.

[15] In total, during various expeditions, Volters and his assistants collected some 1,000 fairy tales, 300 songs, and 2,000 examples of other oral traditions (riddles, proverbs, jokes, etc.).

In 1884, at the Vilnius Public Library, Volters found a copy of the Catechism, or Education Obligatory to Every Christian by Mikalojus Daukša, the first Lithuanian book published in the former Grand Duchy of Lithuania.

Eventually, it was ruled that the press ban did not apply to purely academic publications and Volters was allowed to publish 100 copies of the catechism in 1886.

He made a copy of the history of Lithuania by Simonas Daukantas and convinced Aleksandras Burba [lt], then editor of Vienybė lietuvninkų, to publish the work in the United States.

Volters also edited and prepared for publication the Lithuanian–Latvian–Polish–Russian dictionary (about 15,000 words) written by Mykolas Miežinis [lt] (1827–1888) and published in 1894 in Tilsit (now Sovetsk, Kaliningrad Oblast).

[12] In January 1904, Volters managed to get approval for a small publication (dedicated to the memory of Pranas Vaičaitis) of poems by Russian poets Alexander Pushkin, Mikhail Lermontov, and Aleksey Koltsov translated into Lithuanian.

[3] In 1888–1889, with funding from the Imperial Russian Geographical Society, he surveyed and excavated more than 210 tumuli near Trakai, Lida, Marijampolė, but did not publish his findings.

[21] In 2000, Adolfas Tautavičius published a bibliography of Lithuanian archaeology that included 98 works by Volters though much remains unpublished and scattered among different libraries and archives.