The National Music Museum has a collection of more than a thousand instruments from the 16th to the 20th century, mostly European, but also African and Asian, of both classical and popular traditions. The greater part comes from the former collections of Michel'Angelo Lambertini, Alfredo Keil and Carvalho Monteiro. This includes rare instruments of incalculable historical and organological value and is remarkable due to the quantity and quality of instruments made in Portugal, items rarely found in other comparable museums.

The collection includes several unique items, such as the cors anglais by Grenser, by Grundman & Floth (Leipzig, late 18th century) and by Ernesto Frederico Haupt (Lisbon, mid 19th century); some extremely rare, like the oboe made by Eichentopf (Leipzig, second quarter of the 18th century) and some of enormous organological importance, such as the harpsichord built by Pascal Taskin.

Among the instruments produced in Portugal, particularly noteworthy are the harpsichord built by Joaquim José Antunes (Lisbon, 1758), the 18th-century harpsichords from Lisbon and Oporto workshops, the violins and cellos made by José Galrão (active in Lisbon between 1760 and 1794), the transverse flutes of the Haupt 'dynasty' (mid 18th century to late 19th), the cornets and trombones produced by Rafael Rebelo (Lisbon, 1875), the organ constructed by Joaquim Fontanes (late 18th century) and the guitars by Domingos José Araújo (Braga, 1812).

Several items are important as mementoes of their owners, significant personalities in the Portuguese and European public and cultural lives. Such is the case with the piano (Boisselot & Fils) that Franz Liszt brought from France in 1845; the horn made by Marcel-Auguste Raoux for Joaquim Pedro Quintela, the 1st Count of Farrobo; the Antonio Stradivari cello, that was played and owned by King Luís, and the Henry Lockey Hill cello that belonged to the cellist Guilhermina Suggia.

Others are rather curious, such as the pocket fiddles ('kits', as they were known), used by dancing teachers; the crystal and silver flute; the stick flutes; the mellophone that belonged to Jean Louis Olivier Cossoul and the trumpets marine.

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