Born in La Spezia, Adriano Rimoldi moved to Florence in the 1930s in order to study medicine. As he grew passionate about theatre, he participated in some student spectacles organized by the GUF-Teatro sperimentale and won a radio contest as announcer and newsreader. His first role was that of a radio man in the white telephone comedy Mille lire al mese (Max Neufeld 1939) which starred Alida Valli and which dealt with the new medium of television. Rimoldi's role as protagonist in Addio giovinezza! (1940) by Ferdinando Maria Poggioli, catapulted Rimoldi to stardom. In the film Rimoldi must choose between a simple seamstress (Maria Denis) and a femme fatale (Clara Calamai). In Tosca (1940/41), started by Jean Renoir but finished by Carl Koch, Rimoldi plays the rebel Angelotti, who manages to flee from Scarpia's prison but later on is betrayed by Tosca. He mostly worked with director Corrado D'Errico (Miseria e nobiltà, 1940; La compagnia della Teppa, 1941; Capitan Tempesta, 1942; Il leone di Damasco, 1942) but also with Mario Soldati (Tragica notte, 1942), Dino Falconi (Don Giovanni, 1942), and Christian Jacque (Carmen, 1942; released 1945). It was with Vittorio De Sica's I bambini ci guardano /Children Are Watching Us (1943), that he managed to obtain a substantial lead in a modern, realist drama, as the lover of Isa Pola, wrecking her marriage and family life.
During the time of the German Occupation, Rimoldi worked in Spain, and became a star of in the Spanish cinema. He played leads in films such as Dora la espía (Raffaele Matarazzo 1943) which co-starred the diva of the silent era Francesca Bertini, followed by a dozen films by Ignacio F. Iquino, often paired with Spanish actress María Martín. Rimoldi returned to Italy in the late 1940s in La mano della morta (Carlo Campogalliani 1949) with María Martín, Sigillo rosso (Flavio Calzavara 1950) with Gino Cervi and Carla del Poggio, Capitan Demonio (Carlo Borghesio 1950), again with Martín in the Giovanni Guareschi adaptation Gente cosí (Fernando Cerchio 1950) with Vivi Gioi and Camillo Pillotto, and Ultimo perdono (Renato Polselli 1952) with Franca Marzi. In 1952 Rimoldi returned to theatrical comedy with Gran baldoria by Garinei and Giovannini, and with Isa Miranda in 1955 in Valentino Bompiani's Albertina, directed by Italo Alfaro. In 1954 Rimoldi acted in the new medium of television in three television plays; he also managed to establish himself there with the operetta Wunderbar, directed by Daniele D'Anza. From the late 1950s to the early 1960s Rimoldi played again in several Spanish films and had a recurring role as the cook in the Spanish TV series Cocina (1957-1958). On the big screen, Rimoldi played Melchior in King of Kings (Nicholas Ray 1961) and in 1963 on tv in the drama Nocturne in New York by Clifford Odets. In 1965 Rimoldi enacted his final film role in the Spanish comedy Zarabanda Bing Bing (José María Forqué 1966) starring Jacques Sernas; the same year he died in Rome; Adriano Rimoldi is the maternal grandfather of film director Matteo Garrone.