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• Robert Downey, Jr. as Sherlock Holmes. Downey was visiting Joel Silver's offices with his wife, producer Susan Downey, when he learned about the project.[4] Ritchie initially felt Downey was too old for the role because he wanted the film to show a younger Holmes on a learning curve like Batman Begins.[5] Ritchie decided to take a chance on casting him in the role, and Downey told the BBC that "I think me and Guy are well-suited to working together. The more I look into the books, the more fantastic it becomes. Holmes is such a weirdo".[6] Downey also revealed what his wife had to say: "that when you read the description of the guy  — quirky and kind of nuts — it could be a description of me".[7] Downey intends to focus more on Holmes' patriotic side and his bohemianism, and felt that his work on Chaplin has prepared him for an English accent.[8] Ritchie feels his accent is "flawless".[9] Both Downey and Ritchie are martial arts enthusiasts, and have been inspired by the Bartitsu mentioned in the 1901 story The Adventure of the Empty House.[10] Downey lost weight for the part, because during a chat he had with Chris Martin, Martin recommended that Holmes look "gaunt" and "skinny".[11][12]
• Jude Law as Dr. John Watson, Holmes' ally, a surgeon and a war veteran. Law's Watson is more like the original character, who was more of a colleague, rather than the bumbling fool that actor Nigel Bruce popularized in the 1930s —40s films.[13] Law previously appeared in the Granada Television series The Adventures of Sherlock Holmes, in an episode based on The Adventure of Shoscombe Old Place. Being a Holmes fan, Law recognized there was material unexplored in other adaptations and was intrigued by Downey's casting; Law was cast because he had a positive meeting with Downey and concurred the film would have to explore Holmes and Watson's friendship. Downey believed by emphasizing Watson's qualities as a former soldier, a doctor, a womaniser and a gambler, it would make for a more interesting foil for Holmes.[14] Law made a notebook of phrases from the stories to improvise into his dialogue.[15] Ritchie originally envisioned Russell Crowe in the role.[16]
• Mark Strong as Lord Henry Blackwood, the main antagonist. An aristocrat dabbling in the occult to compel others to do his bidding. Strong works with director Ritchie for the third time and says he appreciates the director's lack of ego and how easy he is to work with.[17][18]
• Rachel McAdams as Irene Adler, a femme fatale from New Jersey who outwitted Holmes twice.[13] In the film, Adler is no longer married to Godfrey Norton and needs Holmes' help for the case.[14] Downey convinced Ritchie to cast McAdams, arguing she would not look too young to be his love interest.[19]
• Kelly Reilly as Mary Morstan. Watson wishes to settle down with her, causing a conflict with Holmes.[7]
• Eddie Marsan as Inspector Lestrade.[20]
• Hans Matheson as Lord Coward, the Home Secretary. Blackwood's right-hand man, who assisted Blackwood in all his murders and was the only one of his allies aware of Blackwood's usage of technology to feign magical powers.
• Geraldine James as Mrs. Hudson, Sherlock Holmes' landlady.
• James Fox as Sir Thomas Rotherham, father of Lord Henry Blackwood and Head of the Four Orders.
• Robert Maillet as Dredger, a French Canadian henchman working for Blackwood.[21]

Director Guy Ritchie declined to say who voiced the character of Professor Moriarty. Rumors suggested that the part was voiced by Brad Pitt, who has been reported to have expressed strong interest in the sequel.[22] Actor Ed Tolputt is credited as "Anonymous Man"[23] although it is not clear if this refers to Moriarty.[24]