There is more than one answer to this question, dependent on your persepctive on life. But the first and most obvious answer, in a modern world, is that it is famous for French wine. It is the largest wine producing region in the world, by hectares, and produces 30% of France's wine output. The 3 biggest AOC's being Corbieres, Minervoise and Cotes du Roussillon, but there are of course many more.
If you are interested in History, on the other hand, then you may consider that the region is most famous for its Albigensian Crusade, otherwise known as the persecution of the Cathars. This crusade was commissioned by Pope Innocent III and he offered the crusaders absolution from their sins, effectively a ticket into heaven, if they joined the crusade for a mere 40 days. The ojective of the crusade was to eliminate Catharism, and it very nearly did. It went on for 46 years during the 13th Century and the most famous leader of the crusade was a gentleman called Simon de Montfort, although that may be an inappropriate use of the term gentleman, because that is something he certainly was not.
Geographically, it is famous for being the neighbor of Provence and for forming a large section of the French Mediterranean coastline that runs from Provence all the way to the Spanish border. Montpellier in the department of Herault is the capital and it is famous for its French cafe culture and vibrant, modern image.
There will be other views on why Languedoc Roussillon is famous and you can read more about the region in the article [Where to go in Languedoc Roussillon] if you are interested.
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