The Vienna Secession was founded in 1897 and became synonymous with Viennese art nouveau. The first significant acquisitions by the Moderne Galerie (from 1903) came from Secession exhibitions and formed the basis of the Belvedere collection. After the art of the fin de siècle found its climax in Gustav Klimt's "Golden Period", early expressionism followed, represented among others by Oskar Kokoschka and Egon Schiele.

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The borderline between symbolism and Secessionism is not always easy to draw. Both trends rejected a naturalist representation of material reality. The main agenda of the symbolists was to express states of mind and soul, irrational forces, dream, ecstasy and vision. Major works of symbolism are The Evil Mothers (1894) by Giovanni Segantini, Half-figure of a Nymph (1896) by Fernand Khnopff and Awe-struckness (1900) by Ferdinand Hodler.

The Secessionists wanted to redesign the whole of life artistically, transform the prosaic everyday into an aesthetic experience. Along with Gustav Klimt, Carl Moll was one of the major exponents of Secession art, as seen in works like Twilight (c. 1900). The close personal connections between the Secession and the Wiener Werkstätte led in 1902 to the Beethoven Exhibition, planned as a "temporary  Gesamtkunstwerk (total work of art)", for which Klimt created the Beethoven frieze. In 1905, a controversy was unleashed about the exclusion of selling activities from the Secession exhibition programme; the "Klimt Group", with Klimt and Moll at its head, left the Secession.

In the same year, the "Brücke" was formed in Dresden and the " Fauves" in Paris. Aestheticism was no longer at the forefront, but the innovative, expressive message that left all academic conventions behind it. In Austria, the works of the young painter Richard Gerstl were among the earliest examples of expressionist tendencies. His painting The Sisters Karoline and Pauline Fey (1905) shows the influence of Edvard Munch. Later pictures manifest the example of Vincent van Gogh, such as the Laughing Self-Portrait (1908), which Gerstl painted shortly before his suicide. Soon afterwards, the young Oska Kokoschka shocked the Viennese public with distressingly forthright portraits.

Egon Schiele, just turned twenty, painted several portraits around 1910 that were remarkable for their piercing urgency and dramatic gesture, arousing deep and disturbing associations. Max Oppenheimer also belonged to the group of early expressionists; his Klingler Quartet (1916) betrays the confrontation between cubists and futurists. A fellow artist very close to Schiele was Anton Faistauer from Salzburg, showing in his emotive Portrait of a Lady in a White Blouse (1913) a similarly unconstrained handling of colour like Anton Kolig’s Portrait of the Wife of the Artists with Flowers (1913). A culmination of this expressive use of colour is seen in the work of the Carinthian painter Herbert Boeckl. His Still Life with Bottles and Fishes (1922) appears as an agitated, pastel configuration that follows its own colour and form structures.