- Clint Eastwood as "Blondie" (a.k.a. the Man with No Name): The Good, a subdued, confident bounty hunter who teams up with Tuco, and Angel Eyes temporarily, to find the buried gold. Blondie and Tuco have an ambivalent partnership. Tuco knows the name of the cemetery where the gold is hidden, but Blondie knows the name of the grave where it is buried, forcing them to work together to find the treasure. In spite of this greedy quest, Blondie's pity for the dying soldiers in the chaotic carnage of the War is evident. "I've never seen so many men wasted so badly," he remarks. He also comforts a dying soldier by laying his coat over him and letting him smoke his cigar. Rawhide had ended its run as a series in 1966, and at that point neither A Fistful of Dollars nor For a Few Dollars More had been released in the United States. When Leone offered Clint Eastwood a role in his next movie, it was the only big film offer he had; however, Eastwood still needed to be convinced to do it. Leone and his wife traveled to California to persuade him. Two days later, he agreed to make the film upon being paid $250,000 and getting 10% of the profits from the North American markets—a deal with which Leone was not happy. In the original Italian script for the film, he is named "Joe" (his nickname in A Fistful of Dollars), but is referred to as Blondie in the Italian and English dialogue.
- Lee Van Cleef as Angel Eyes: The Bad, a ruthless, unfeeling, and sociopathic mercenary who always finishes a job he is paid for (which is usually finding—and killing—people). When Blondie and Tuco are captured while posing as Confederate soldiers, Angel Eyes is the Union sergeant who interrogates and has Tuco tortured, eventually learning the name of the cemetery where the gold is buried, but not the name on the tombstone. Angel Eyes forms a fleeting partnership with Blondie, but Tuco and Blondie turn on Angel Eyes when they get their chance. Originally, Leone wanted Enrico Maria Salerno (who had dubbed Eastwood's voice for the Italian versions of the Dollars Trilogy films) or Charles Bronson to play Angel Eyes, but the latter was already committed to playing in The Dirty Dozen (1967). Leone thought about working with Lee Van Cleef again: "I said to myself that Van Cleef had first played a romantic character in For a Few Dollars More. The idea of getting him to play a character who was the opposite of that began to appeal to me." In the original working script, Angel Eyes was named "Banjo", but is referred to as "Sentenza" (meaning "Sentence" or "Judgement") in the Italian version. Eastwood came up with the name Angel Eyes on the set, for his gaunt appearance and expert marksmanship.
- Eli Wallach as Tuco Benedicto Pacífico Juan María Ramírez (known as "The Rat" according to Blondie): The Ugly, a comical and oafish but cagey and resilient, fast-talking Mexican bandit who is wanted by the authorities for a long list of crimes. Tuco manages to discover the name of the cemetery where the gold is buried, but he does not know the name of the grave. This state of affairs forces Tuco to become reluctant partners with Blondie. The director originally considered Gian Maria Volontè for the role of Tuco, but felt that the role required someone with "natural comic talent". In the end, Leone chose Eli Wallach, based on his role in How the West Was Won (1962), in particular, his performance in "The Railroads" scene. In Los Angeles, Leone met Wallach, who was skeptical about playing this type of character again, but after Leone screened the opening credit sequence from For a Few Dollars More, Wallach said: "When do you want me?" The two men got along famously, sharing the same bizarre sense of humor. Leone allowed Wallach to make changes to his character in terms of his outfit and recurring gestures. Both Eastwood and Van Cleef realized that the character of Tuco was close to Leone's heart, and the director and Wallach became good friends. They communicated in French, which Wallach spoke badly and Leone spoke well. Van Cleef observed, "Tuco is the only one of the trio the audience gets to know all about. We meet his brother and find out where he came from and why he became a bandit. But Clint's and Lee's characters remain mysteries." In the theatrical trailer, Angel Eyes is referred to as The Ugly and Tuco, The Bad. This is due to a translation error; the original Italian title translates to "The Good [one], the Ugly [one], the Bad [one]".
- Aldo Giuffrè as Captain Clinton
- Mario Brega as Corporal Wallace
- Luigi Pistilli as Father Pablo Ramírez
- Al Mulock as Elam
- Antonio Casas as Stevens
- Antonio Casale as Bill Carson/Jackson
- Antonio Molino Rojo as Captain Harper
- Rada Rassimov as Maria
- Enzo Petito as Storekeeper
- Chelo Alonso as Stevens' Wife
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