He later joined the faculty of the University of Genoa and, while there, translated French literature. With a colleague, he prepared a six-volume dictionary of mythology and antiquities, including the Celtic history in Italy. Romani's expertise in French and antiquity is reflected in the libretti he wrote; the majority are based on French literature and many, such as Norma, use mythological sources.

Romani travelled widely in Spain, Greece, Germany, and France. In 1814, he established himself in Milan, where he became friends with important figures in the literary and musical world. He turned down the post of court poet in Vienna, and began instead a career as opera librettist. He wrote two librettos for the composer Johann Simon Mayr, which resulted in his appointment as the librettist for La Scala. Romani became the most highly regarded of all Italian librettists of his age, producing nearly one hundred. In spite of his interest in French literature, he refused to work in Paris.

As a rule, Romani did not create his own stories; he kept up with what was happening in the Paris theatre and adapted plays which were popular there, but this wasn't always a safe strategy, given the vague intellectual property rights legislation of the time. In one case, Romani prepared a libretto based on the play Lucrezia Borgia by Victor Hugo for the opera Lucrezia Borgia by Donizetti, but when it was staged in Paris in 1840, Hugo obtained an injunction against further productions. The libretto was then rewritten and retitled La Rinegata, with the Italian characters changed to Turks.

Romani wrote the librettos for Bellini's Il pirata, La Straniera, Zaira, I Capuleti e i Montecchi, La Sonnambula, Norma and Beatrice di Tenda, for Rossini's Il Turco in Italia and Bianca e Falliero, and Donizetti's Anna Bolena and L'elisir d'amore (which he adapted from Eugene Scribe's Le philtre). He also wrote a libretto (originally for composer Adalbert Gyrowetz) that Verdi used for his early comedy Un giorno di regno.

Romani was considered an ideal match for Bellini, who is quoted as having said: "Give me good verses and I will give you good music". Dramatic, even extravagant "situations" expressed in verses "designed to portray the passions in the liveliest manner" was what Bellini was looking for in a libretto, according to a letter to Florimo, August 4, 1834, and he found them in Romani.

The two, however, had a falling out over missed deadlines for Beatrice di Tenda.. After setting I Puritani to a libretto by Carlo Pepoli, Bellini was determined not to compose any more Italian operas with anyone but Romani. I Puritani was his last opera; he died less than a year after its première. Romani mourned him deeply and wrote an obituary in which he expressed his profound regrets over their disagreement.

In 1834 Romani became editor of the Gazzetta Ufficiale Piemontese to which he contributed literary criticism. He retained the post, with a break 1849—1854, until his death, in Moneglia, (in the region of Liguria, Italy). A volume of his lyric poems was published in 1841.

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