Was first trained in science (BA, Harvard, in molecular biology), then in comparative literature, at Brown University, from which he received his Ph.D., specializing in narratology and the modern novel. He is the author of articles on several 20^thCentury American novelists, especially Thomas Pynchon; he was also the co-founder and co-editor of a journal devoted to the study of his work, Pynchon Notes, published from 1979 to 2009.

Tölölyan also published numerous articles on cultural and social issues of the Armenian diaspora in the Paris newspaper Haratch, some of which were published in 1980 as a book, Spyurki Mej.

In the 1980s, Tölölyan published a number of articles on Armenian terrorism committed by diaspora Armenians, and in 1991 he was the founding editor of a periodical titled Diaspora: a journal of transnational studies, which is generally considered the foundational publication for the emerging discipline of diaspora studies, launched by the Oxford University Press and, since 1996, published by the University of Toronto Press. The journal publishes articles on both classical and newly emergent diasporas, as well as on the theoretical issues pertaining to diaspora studies and, finally, on the relations of diasporas with ethnicity, nationalism, migration and postcolonialism.