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George Lois, the hard-selling, charismatic advertising man and designer who fashioned some of the most daring magazine images of the 1960s and popularized such catchphrases and brand names as “I Want My MTV” and “Lean Cuisine,” has died. He was 91.

Lois’ son, the photographer Luke Lois, said he died “peacefully” Friday at his home in Manhattan.

Nicknamed the “Golden Greek” and later (to his displeasure) an “Original Mad Man,” George Lois was among a wave of advertisers who launched the “Creative Revolution” that jolted Madison Avenue and the world beyond in the late 1950s and ’60s. He was boastful and provocative, willing and able to offend, and was a master of finding just the right image or words to capture a moment or create a demand.

His Esquire magazine covers, from Muhammad Ali posing as the martyr Saint Sebastian to Andy Warhol sinking...