The following year he exhibited for the first time, showing paintings inspired by the works of Walter Scott and Machiavelli at the Florentine Promotrice.
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Among his most notable paintings are The Ward of the Madwomen at S. Bonifazio in Florence (1865, Venice, Gallery of Modern Art in Cà Pesaro); Bagno Penale a Portoferraio (ca. 1890, Florence, Gallery of Modern Art in Palazzo Pitti), which portrays the well-known brigand Carmine Crocco during his imprisonment; and Leith (1881, Florence, Gallery of Modern Art in Palazzo Pitti).
In Florence she knit lasting friendships with the painter Telemaco Signorini and the learned Mario Praz, and she encouraged his love of learning and English literature.
Carlo Felice Biscarra, and Luigi Rocca published a monthly journal with engraved works of art titled L'arte in Italia (1869–1873), which used Bignami, along with Telemaco Signorini and N. Costa, as engravers.
Macchiaioli painters who dedicated time to Castiglioncello included Giovanni Fattori, Silvestro Lega and Telemaco Signorini, among others.