Between 1840 and 1872, he held a number of teaching and administrative positions in his order's educational institutions in Venice and Paris.

During this period, he gained renown as a poet, writing mainly in Classical Armenian on both patriotic and religious themes.

He notably wrote a number of long works on the historical provinces of Armenia and prepared for publication many old Armenian texts.

[2][3] From 1841 to 1850, he worked as a teacher and, from 1848, principal at the Raphael College (the Mekhitarist-run Armenian boarding school) in Venice.

[4] Alishan was a prolific author who wrote across different genres over the course of his more than sixty-year-long career․[5][6] He began his literary career in 1843, publishing works in prose and verse and scholarly articles in Bazmavep.

Alishan gave up poetry in his early thirties, announcing his departure from the genre with the poem "Husk ban ar Vogin nvagahann" (A final word to the singing Spirit).

His patriotic poems emphasize the concept of homeland, its natural beauty, and heroic episodes in Armenian history.

One of his poems was later set to music by the Venetian violinist Pietro Bianchini and given the title "Bam porotan" (Boom, they roar).

Most Soviet Armenian authors, on the other hand, celebrated the "Ergk Nahapeti" over the rest of Alishan's poems.

[8] Alishan translated works in prose and verse from English, French, Persian and Italian into Armenian.

[6] Alishan planned to complete 20–22 large volumes on the provinces and districts of historical Armenia, but published only four: Shirak (1881), Sisuan (1885), Ayrarat (1890) and Sisakan (1893).

These include a collection of Armenian folk songs translated into English (1852), a collection of primary sources in Italian regarding Armeno-Venetian relations in the medieval period (L'Armeno-Veneto, 1893), and several French adaptations of his Armenian studies, such as Étude de la patrie: Physiographie de l’Armenie (1861), Schirac, canton d’Ararat (1881), and Sissouan, ou l’Arméno-Cilicie: description géographique et historique (1899).

[1][7] According to Bardakjian, "Any search [in Alishan's work] for dissension from Christian tenets on the Creator, the Creation, and human behavior would be a futile attempt.

"[7] Alishan rooted his understanding of Armenian history in the biblical narrative of Genesis and tried to prove the traditional view that the Garden of Eden was located in Armenia using data from modern science.

He suggests that the "boisterous tone" in some of Alishan's poems may "replace, or cover up, rebellious sentiments unutterable by a monk.