Helene Müller was born on 11 February 1869 in Horst, near the German city of Essen, the third child of Wilhelm Müller and Emilie Neese. In 1876 the Müller family moved to Düsseldorf. Wilhelm Müller was involved in the sale of mining and blast furnace products and started his own company, Wm. H. Müller & Co. Two years later he opened a branch in Rotterdam, managed by Willem Kröller.
It was in around 1882 when Anton Kröller, the youngest brother of Willem Kröller, first became acquainted with the Müller family. He stayed with them while learning the ropes at Wm. H. Müller & Co. In 1887, 18-year-old Helene and Anton Kröller met once again in her father’s office. In 1888 they were married and settled in Rotterdam.
In 1889 Anton Kröller became the head of the firm. Under his leadership the company grew into a powerful international concern with major interests in shipping, the American grain trade and ore mining in North Africa and Spain. The headquarters of Wm. H. Müller & Co. was located on the Lange Voorhout in The Hague.
Between 1889 and 1897 the couple had four children: Helene, Toon, Wim and Bob. For many years the Kröllers lived in The Hague, but in early 1916 they moved to Wassenaar. Later they also lived for a few years in the St Hubert Hunting Lodge, which was located in the middle of the Veluwe region and had been designed by H.P. Berlage. Anton Kröller, an enthusiastic hunter, purchased a few farms there over the years as well as 6,000 hectares of woodland and moorland.
In 1938 the Rijksmuseum Kröller-Müller was opened in the middle of this nature reserve. Helene Kröller-Müller died in 1939 at age 70. Anton Kröller died two years later. Both are buried on the Franse Berg (French Hill), near the museum.