'The Hound of the Baskervilles' (1902) is widely considered the most popular and famous Sherlock Holmes story. It combines detective work with Gothic horror elements and has been adapted numerous times for film and television. While 'A Scandal in Bohemia' (Option A) introduced Irene Adler and 'The Final Problem' (Option C) featured Moriarty, Baskervilles remains the most widely recognized and adapted story.