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Alboni was born at Città di Castello, in Umbria. She became a pupil of Antonio Bagioli of Cesena, Emilia–Romagna, and later of the composer Gioachino Rossini, when he was 'perpetual honorary adviser' in (and then the principal of) the Liceo Musicale, now Conservatorio Giovanni Battista Martini, in Bologna. Rossini tested the humble thirteen-year-old girl himself, had her admitted to the school with special treatment, and even procured her an early engagement to tour his Stabat Mater around Northern Italy, so that she could pay for her studies. After she achieved her diploma and made a modest debut in Bologna, in 1842, as "Climene" in Pacini's Saffo, she obtained a triennial engagement thanks to Rossini's influence on the impresario Bartolomeo Merelli, Intendant at both Milan's Teatro alla Scala and Vienna's Imperial Kärntnertortheater. The favourable contract was signed by Rossini himself, "on behalf of Eustachio Alboni", father of Marietta, who was still a minor. The singer remained, throughout her life, deeply grateful to her ancient "maestro", nearly a second father to her.
Her debut at Teatro alla Scala took place in December 1842 as "Neocle" in the Italian version of Le siège de Corinthe, which was followed by roles in operas by Marliani, Donizetti (as "Maffio Orsini" and "Leonora" in the Scala premiere of an Italian version of La favorite), Salvi and Pacini. In the season 1844–1845 she was engaged in the Saint Petersburg Imperial Bolshoi Kamenny Theatre; later, in 1846–47, she toured the principal cities of Central Europe, finally reaching London and Paris, where she settled permanently. In London, "she appeared in leading roles by Rossini and Donizetti (where she outshone Giulia Grisi and Jenny Lind) and also sang Cherubino (performing with Henriette Sontag)". For the 1848 London run of Les Huguenots, Meyerbeer transposed the role of the page "Urbain" 'from soprano to contralto and composed the aria "Non! – non, non, non, non, non! Vous n'avez jamais, je gage" in Act 2' for her. On 28 August 1848, she sang at a concert in Manchester's Concert Hall, sharing the stage with Lorenzo Salvi and Frédéric Chopin. She toured the United States in 1852–53, appearing there with Camilla Urso.