He first visited Paris in 1898 and then moved there in 1899, where he attended the École des Beaux-Arts and took classes at the Académie Julian. It took just two years for him to develop his characteristic style, and soon he was exhibiting his paintings at the Salon des Indépendants and the Salon d'Automne. Tarkhoff was increasingly influenced by Van Gogh and Post-Impressionism, as evidenced by his typical choice of subjects-rural landscapes and floral still life compositions and his thick impasto.

Tarkhoff was notably recognized as one of the first pioneers of Fauvism, alongside such well-known French painters Henni Matise, Maurice de Vlaminck, and André Derain. Their style was evidently indebted to Impressionistic tenets, for it often emphasized varying qualities of light as well as broad, visible brushwork, yet their paintings explored a unique and powerful expression of energy, the potent force of pure color. At the Salon d'Automne of 1907, Tarkhoff's exuberant palette led one reviewer to regard him as "part of the younger Bohemian crowd [who] outrage even the Byzantines and our North American Indians with their brilliant color" (as quoted in Eleanor Green, Nicolas Tarkhoff, Berry-Hill Galleries, 1989, p. 7).

His artwork was deemed innovative and extraordinarily desirable, so much so that Tarkhoff was granted solo exhibitions at Galerie Ambroise Vollard (where Gauguin, Cézanne, and Renoir had all exhibited) in 1906 and Galerie Drouet in 1909. As early as 1910, an impressive list of collectors had acquired his work, including Ambroise Vollard, Sergei Shchukin, Vladimir Girshman, and many others.