Joining him in his studies were Yosef Kohjinoff, Rafael Potihaloff, Moshe Cheh Yizhakoff, Avraham Aminoff Talmudi, and Aba Shimon Gaon.

In 1888, motivated by religious convictions, he made aliyah to Palestine and was one of several Bukharan Jews responsible for founding the new Jerusalem neighborhood of Rehovot HaBukharim[1] (later shortened to Bukharim) in 1891.

He has kept me alive, and has brought me to the place of my desire for the good life and peace to see the pleasantness of God and to visit his sanctuary.

Prayer to God is what connects Israel to their Father in Heaven, although the Israelite nation has been vanquished in exile for more than eighteen hundred years".From the late 19th century until World War I, the Bukharim neighborhood was one of the most affluent sections of the city, populated by Bukharan Jewish merchants and religious scholars supported primarily by various trading activities such as cotton, gemstones, and tea in Central Asia and Russia.

Shlomo Moussaieff married Esther Gaonoff, who traced her ancestry to Yosef Maimon, originally of Tetuan, Morocco, who arrived in Bukhara in the late 18th century and revived Rabbinic learning there.

Their daughter, Miriam, married Mullah Pinhas Hakatan (d. 1875), a renowned Rabbi, called by the missionary and traveler, Joseph Wolff, "the most learned of the Jews of Bukhara" and "a young man of extraordinary talents".

The members of the group, however, consulted with the guide who told them that the area they were in was inhabited by dangerous animals and they must leave immediately for safer ground.

He died in 1910 in Jerusalem.Moussaieff and his wife had seven children: Yehuda, Sam, Henri,[8] Maurice, Rehavia (who was named after the neighborhood Moussaieff helped found, Rehovot HaBukharim,[4] Sarah, and Bat Sheva.

His son Sam (Shlomo), a self made millionaire, bought the Aleppo Codex and brought it to Israel.

Much of his property in the Bukharim quarter was declared a "religious endowment" (hekdesh in Hebrew and waqf in Arabic), which could not be sold for perpetuity.

Till this day, proceeds from rentals of his property are received by the direct male descendants of Moussaieff who live in Israel.