Bob and Mike Bryan beat Ivan Dodig and Marcelo Melo to become the first pair to hold all four Grand Slam doubles titles simultaneously in the Open era.
The American twins, also the reigning Olympic champions, stayed on course for a calendar Grand Slam with their 3-6 6-3 6-4 6-4 victory on Centre Court.
Ken McGregor and Frank Sedgman are the only team to win all four Grand Slam titles in the same year, in 1951.
It was the Bryans' third Wimbledon title and 15th major title in total.
The Bryans, 35, won their sixth Australian Open title earlier this year before securing their second French Open title last month.
Mike Bryan said: "It's hard to even dream that we'd have the slam, all four at one time. It all started back after we won the gold. It just felt like a huge pressure was released. We went on to win the Open and had a great summer.
"This year we've been on an amazing run - never had a streak like this."
Were they to win their fifth US Open title in September they would be the first team since Australia's McGregor and Sedgman 62 years ago to win all four major tournaments in the same year.
Croatia's Dodig, 28, and Brazil's Melo, 29, were bidding to win their first Grand Slam doubles title in what was their first major final.
Bob Bryan put their success down to making sure tennis did not dominate their lives.
"We've been working hard and taking care of our bodies. We've put the game in the right perspective in our life. When we lose, it's not the end of the world.
"He's married; I have a family; I have a kid. We're just playing for fun. We've done it all in the sport, and now we're just out there taking swings and not living and dying with every win and loss."
Su-Wei Hsieh of Taiwan and China's Peng Shuai took the ladies' doubles title with a straight-sets win over the Australian duo Ashleigh Barty and Casey Dellacqua.
The number eight seeds took the first set on a tie-break before completing their first Grand Slam win 7-6 (7-1) 6-1 in 96 minutes.
Meanwhile, Britain's Kyle Edmund and his Portuguese partner Frederico Ferreira Silva lost to French/Italian pair Enzo Couacaud and Stefano Napolitano in the semi-finals of the boys' doubles.
The 18-year-old Edmund, who lost in the semi-finals of the boys' singles, and Silva went down 6-4 7-6 (9-7).