Alexei Harlamoff was born into a family of serfs on 18 October 1840 in the village of Dyachevka near Saratov on the River Volga.

In 1862 Harlamoff was awarded a second class silver medal for a sketch, and he enrolled with the historical painter Alexey Tarasovich Markov.

In 1865 he presented his large scale painting Ananias before the Apostles, but did not win the competition for a second class gold medal.

He spent September and October of that year in Normandy and the southern Netherlands with Alexey Bogolyubov, C. Huhn, and A. Lavezzari.

The conference secretary of the Academy of Arts, Peter F. Iseyev, rejected Bogolyubov's request to grant Harlamoff a professorship.

In December Bogolyubov reported to the council of the Imperial Academy of Arts on Harlamoff's visible success under the guidance of Bonnat.

From April onwards Harlamoff joined the drawing evenings at Bogolyubov's residence in rue de Rome, 95.

He was frequently invited for dinner with Louis Viardot and Pauline Viardot-Garcia in rue Douai 50, where Turgenev occupied the top floor.

In June Harlamoff painted a portrait of Tsar Alexander II in Bad Ems, possibly spending the rest of the summer in Spain.

In May he exhibited at the Salon, where the portraits of Pauline Viardot-Garcia and Louis Viardot drew the attention of the Parisian press.

In 1876 the young soprano singer Félia Litvinne arrived from Saint Petersburg and started taking lessons with Pauline Viardot-Garcia.

In 1885 he supported Bogolyubov's plan to found a museum in Saratov by donating his painting Italian Girl with a Lizard.

At the 19th Itinerant Art Exhibition in Saint Petersburg Tsarina Maria Fedorovna purchased his painting Portrait of a Young Girl.

When Bogolyubov died in 1896 Harlamoff was nominated chairman of the Association of Russian Artists for the Mutual Support and Benefaction with its seat in Paris.