The 30-year-old Hewitt, playing his first match since September in his latest comeback from a bad toe injury, produced a superb second set before world number 24 Verdasco took their match 6-3 3-6 7-5 victory in 128 minutes.
Hewitt's team mate Jarmila Gajdosova defeated Anabel Medina Garrigues 6-3 3-6 6-3 in the women's singles but third-seeded Spain won the mixed doubles 6-3 3-6 (11-9).
Hopman Cup rules state that the third set in the mixed doubles is decided by a tiebreak in which the first pair to reach 10 points with an advantage of two take victory.
Hewitt has not won a major title since Wimbledon in 2002 and has plummeted to number 186 in the rankings.
Despite being a constant subject of retirement speculation, Hewitt refuses to accept that the injury to his left big toe makes it impossible to scale the heights again.
He was quick against Verdasco in the Group B encounter, clawing back from a break down in the final set to ensure a grandstand finish in front of a full house of more than 7,000 at the Burswood Dome.
A third-set tiebreaker was on the cards until consecutive double faults and an errant backhand from Hewitt handed the win to Verdasco.
TOUGH PLAYER
"I just want to play pain-free this year and hopefully finish my career in a good way over the next couple of years," Hewitt said.
"I feel pretty good tonight - we have a day off then we're back out here on Tuesday night. Maybe I should just chop the foot off."
Verdasco praised Hewitt's tenacity, saying: "Lleyton is a very tough player.
"I was playing very well but I still wasn't able to shake him off. He's always there. He's a good friend and I really hope he has a good 2012 with no more injuries.
"It's my first match since we won the Davis Cup and that is still an unbelievable result to me," Verdasco added. "It was an honor to be part of that."
Gajdosova had given the host nation a dream start with a powerful performance in her Hopman Cup debut on the second day of the annual team competition.
"First match of the year, I'm glad it's over," the world number 33 said.
"I wanted to give Lleyton a good start and give us something to build on as a team. A few winners here and there, a few errors, but it turned out well.
"The mixed was fun, Lleyton did everything, he's the superstar. Unfortunately we couldn't quite get over the line."
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