It was the second consecutive year that the show, which ended last September after five seasons, had picked up the ceremony’s highest honor.
Breaking Bad star Bryan Cranston was named best actor in a drama series for a fourth time as the teacher-turned-drug kingpin Walter White.
He beat a host of Hollywood heavyweights including Oscar winner Matthew McConaughey and Woody Harrelson for their roles in the acclaimed crime drama True Detective.
His co-stars Aaron Paul and Anna Gunn were also honored for best supporting actor and supporting actress in a drama series.
British drama Sherlock has won a hat-trick of awards at the Primetime Emmys in Los Angeles.
There were four awards for Sherlock including best cinematography, music, single-camera picture editing and sound editing.
Benedict Cumberbatch and Martin Freeman won best actor and best supporting actor in a mini-series, although neither was at the ceremony.
Steven Moffat also won best writing in a mini-series for the final episode of Sherlock‘s third season.
In other categories, The Good Wife star Julianna Margulies won the Emmy for best lead actress in a drama series for her part as lawyer Alicia Florrick.
There were also best actress and best supporting actress in a mini-series awards for Oscar winners Jessica Lange and Kathy Bates for their roles in American Horror Story: Coven.
Sitcom Modern Family was named best comedy series for a fifth consecutive year, equaling the record set by 1990s show Frasier for most comedy wins.
Ty Burrell also walked away with best supporting actor in a comedy for his role on the show.
The Big Bang Theory‘s Jim Parsons won best actor in a comedy series. Julia Louis-Dreyfus won her third consecutive Emmy for playing foul-mouthed US Vice President Selina Meyer in political satire Veep.
Allison Janney won the best supporting actress in a comedy series for Mom.
The ceremony also paid tribute to industry members who died in the past year.
They included James Garner, Ruby Dee, Sid Caesar, Carmen Zapata and Elaine Stritch.
It concluded with a special homage to Robin Williams by long-time friend Billy Crystal, who remembered the actor as “the brightest star in a comedy galaxy”.
“It is very hard to talk about him in the past because he was so present in our lives,” Billy Crystal said.
“While some of the brightest of our celestial bodies are actually extinct now, their energy long since cool, but miraculously, because they float in the heavens so far away from the sound, their beautiful life will continue to shine on us forever.
“And the glow will be so bright, it will warm your heart, it will make your eyes glisten, and you’ll think to yourself, Robin Williams – what a concept.”
The main ceremony at the Nokia Theatre followed the Creative Arts Emmy prize-giving on August 16, honoring TV guest stars and behind-the-scenes crew.
The 66th Annual Primetime Emmy Awards took place at Nokia Theatre L.A. Live on August 25.
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