His father, Solomon Pimsleur, was a Jewish immigrant from France[2] and a composer of music; his American-born mother, Miera, was a librarian at Columbia University.

After leaving UCLA, Pimsleur went on to faculty positions at the Ohio State University, where he taught French and foreign language education.

He was a Fulbright lecturer at the Ruprecht Karls University of Heidelberg in 1968 and 1969 and a founding member of the American Council on the Teaching of Foreign Languages (ACTFL).

[3] In the period from 1958 to 1966, Pimsleur reviewed previously published studies regarding linguistic and psychological factors involved in language learning.

This led to the publication in 1963 of a coauthored monograph, Underachievement in Foreign Language Learning, which was published in the International Review of Applied Linguistics.

Through this research, he identified three factors that could be used to calculate language learning aptitude: verbal intelligence, auditory ability, and motivation.