The shock decision was announced by England chairman of selectors David Graveney at a post-match news conference at Edgbaston.
Hussain will be replaced by Michael Vaughan, who had already taken over the one-day team from him and led England to victory in the recently concluded triangular series against Zimbabwe and South Africa.
"I just feel it's time for a change," said Hussain, who will continue in the England side as a specialist batsman. "Michael Vaughan has shown in the last few months that he is a very capable leader.
"I think there are some young lads in there who will play under him and the last thing they want is a tired leader.
"I have been thinking about it since the World Cup, to be honest. It's not a knee-jerk reaction, I've been thinking about it for a while."
Hussain, 35, stepped down as national one-day captain after the unsuccessful World Cup campaign in South Africa this year before leading England to a 2-0 series victory over Zimbabwe.
But he had said he wanted to continue captaining at Test level in the hope of breaking the England record for Test wins.
DECISION PROMPTED
He conceded his decision had also been prompted by watching Vaughan captain the one-day side in his place during the recent triangular series.
"Vaughnie and the boys seemed to enjoy those one-dayers," the right-handed batsman said. "My style of captaincy has been about aggression and I believe you have to give them a kick up the backside now and then.
"After seeing a young side enjoy themselves so much and have a different style of captain, it was very difficult on my first day back to be something different ... it had moved on a bit."
South Africa captain Graeme Smith responded by saying he knew something was wrong with England during the game at Edgbaston.
"They (England) were a touch quieter than I expected, I don't know what caused that. Probably that was because they were on the back foot all the time.
"This could be a big breakthrough for us -- it will definitely put a bit of pressure back on Vaughan."
Hussain took over from Alec Stewart as captain in 1999, getting away to a bad start when his team lost a home series to New Zealand.
INSTILLED GRIT
But he soon instilled his own grit and determination into the team, who recorded their first series victory over West Indies since 1969 as well as winning difficult away series in Sri Lanka and Pakistan.
That run of victories, said Hussain, would be one of his personal highlights.
On the reverse side, there were also two heavy losses in Ashes series against Australia.
In total, he captained England 45 times with 17 wins, 15 defeats and 13 draws. Mike Brearley won 18 Tests for England while Peter May held the record with 20.
"It's time for a change," Hussain said. "There's only so many times you can go to the well in terms of digging deep for your team.
"I've tried to play these mental games but I found myself out there on Thursday and I wasn't quite the captain England needed. I wasn't quite on the boil."
Hussain, who was named in an unchanged team on Monday for the second Test at Lord's starting on Thursday, said he wanted to continue playing Test cricket.
Unlike Vaughan, however, his batting position is not guaranteed. He made one and 23 not out in the first Test, while Vaughan made 156 and 22.
"Basically I just want to think about being a batsman, picking my bat up and going out and batting.
"If I am good enough, I will stay in the England side," he added. "If not, someone else can do it."
