The painting collection of the Museum consisted of an initial nucleus coming from the Colegiada de Nossa Senhora da Oliveira, a group of paintings transferred from other extinct convents or chapels of the region and some deposits made in ulterior dates.

The nucleus of the Collegiate Church comprised altarpieces or panels that the successive reforms of the church and of the cloister removed from their original locations and other paintings that were hidden and abandoned, such as the Triptych of the Lamentation and Our Lady with Child.

Between 1929 and 1940, a group of pictorial works, almost all coming from ancient convents or from chapels dependent on the Collegiate Church and that were in the ownership of the State, entered into the Museu de Alberto Sampaio. This group includes, for example, the panels of Virgin and Child (Maria Lactans) between Saint Benedict and Saint Jerome and a Saint Michael, coming from the Igreja de São Miguel do Castelo, and a Saint Gregory the Great, from the parochial church of São Cipriano de Tabuadelo.

As far as the nucleus of deposits is concerned, one may mention two examples: the City Hall of Guimarães deposited in the Museum the Pentecost, which had been part of the small oratory of the old City Hall and the Museu Nacional de Arte Antiga deposited a panel from the 16^th century, by Friar Carlos, depicting Saint Vincent, Saint Martin and Saint Sebastian that had belonged to the Mosteiro de Santa Marinha da Costa.

Providing the counterpoint to the painting on panels, the sculpture collection, in stone or in wood, is also exhibited. These pieces date from the 14^th to the 17^th centuries and a significant part of them come from the Collegiate Church of Guimarães or from other religious institutions of the city.