When Irmgard Neuman discovered that there was a celebrity artist living next door, she bought a book of his work, and, rather boldly, asked him to sign it. Marc Chagall, the pioneer of Modernism, went one better.

Not only did he oblige the autograph-hunter and her husband with their own personalised illustration on the inside leaf, he continued to decorate pages of their books for the next 30 years.

Russian and Israeli art collectors are now circling as the compendium, bearing the stamp of one of the most celebrated artists of the 20th century, is prepared for sale for the first time.

The collection of 49 illustrated texts spans the 30-year friendship between Chagall and his neighbours in Saint-Paul de Vence, the medieval town in the French Riviera, where he settled after the Second World War.

They also feature many of the signature images, from fiddlers, floating brides and life in the shtetl, that led to Chagall’s reputation as “the quintessential Jewish painter of the 20th century”. Together, the books are valued at £250,000-£300,000.

“It would have been like going up to the biggest celebrity artist of today, for example, Damien Hirst, and asking him to do 50 works for free,” Alexander Hayter, of Bloomsbury Auctions, said. “It was done very much as a personal favour, and doesn’t happen very often. They were obviously very close. Every couple of weeks, they would meet up for tea, and Chagall would do a drawing for them. As he got to know them better, the drawings became more elaborate.”

They range from simple pen and ink sketches to vivid watercolours, depicting many of the same images from Yiddish folklore celebrated in the most famous works by Chagall, born Mark Zakharovich Shagal to a poor Hassidic family in 1887 in Belarus.

They are incorporated with lithographs, biographies and art history books about Chagall. Even the artist himself was proud of the Neuman archive. “He took a personal interest in it, and was delighted to see it grow,” Mr Neuman recalled, before his death. “You know,” he would say, “this collection is unique.”

Shielded from public view, the books were eventually bequeathed to the Leo Baeck College, London, in 1993, where they were archived among the private collection of ancient Hebrew texts and religious scriptures.

The college, which was one of the first seminaries in Britain to provide training for rabbis, has decided to sell the collection to raise funds for its training programmes, which send scholars to teach across Europe.

Also included is a portfolio of unpublished photographs, taken by Mr Neuman between 1974 and 1984, depicting the artist in his studio towards the end of his career.

The collection will be sold at auction on January 29.

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