Vester Lee Flanagan, 41, a former employee of WDBJ7 TV known professionally as Bryce Williams, was in a car that was surrounded by police following a chase.
WDBJ7 TV reporter Alison Parker and cameraman Adam Ward were killed some seven hours earlier during an interview in the town of Moneta.
Vester Lee Flanagan later uploaded a video of himself opening fire at close range.
The White House has urged Congress to rapidly pass gun control laws in the wake of this latest shooting in the US.
Virginia State Police said Vester Lee Flanagan’s car had been spotted on I- 66 following the shooting, and crashed off the road after being pursued by officers.
“Troopers approached the vehicle and found the male driver suffering from a self-inflicted gunshot wound,” the force said in a statement.
The suspect later died in hospital, a police spokesman said.
Vester Lee Flanagan’s Twitter account suggested he had held a grudge against Adam Ward, 27, and Alison Parker, 24.
Police said his utterances on social media the previous evening suggested the attack was pre-planned.
The attack on the journalists took place at a large shopping centre, Bridgewater Plaza, near Smith Mountain Lake.
Alison Parker was starting a breakfast TV interview about tourism at the shopping centre when suddenly shots rang out, the camera spun and dropped to the ground, and her screams could be heard.
The footage then captured what appeared to be a fleeting image of the gunman, who was wearing black trousers and a blue top – and holding a handgun.
The woman who was being interviewed, later identified as Vicki Gardner of the Smith Mountain Lake Regional Chamber of Commerce, survived the attack and is in a stable condition in hospital following surgery.
Bryce Williams’s Twitter and Facebook feeds, which have now been suspended, subsequently showed video shot by the gunman.
Videos showed him raising a handgun, training it on the trio, and opening fire 14 times. The TV station’s own footage of the attack recorded only eight of the shots.
Staff at the WDBJ7 TV, which continued broadcasting after the live report, expressed shock and sadness at the loss of their colleagues.
The station’s president and general manager, Jeffrey Marks, announced on air: “Alison and Adam died this morning at 06:45 shortly after the shots rang out.
“I cannot tell you how much they were loved by the WDBJ7 team… our hearts are broken.”
Jeffrey Marks described Bryce Williams as “an unhappy man” who was “difficult to work with” and had to be escorted from the TV station by police officers when he was finally dismissed.
A complaint filed against the station with the Equal Employment Opportunity Commission by the suspect had been dismissed, Jeffrey Marks added.
WDBJ7 anchor Chris Hurst revealed that he and Alison Parker had been in a relationship and had planned to marry.
“We were together almost nine months. It was the best nine months of our lives. We wanted to get married. We just celebrated her 24th birthday.
“She was the most radiant woman I ever met. And for some reason she loved me back. She loved her family, her parents and her brother.”
Chris Hurst added that Alison Parker had worked on a regular basis with Adam Ward, and that he was heartbroken for his fiancée, a producer at the station.
White House spokesman Josh Earnest, speaking to reporters, urged the passing of new gun control laws.
“There are some common sense things that only Congress can do that we know would have a tangible impact on reducing gun violence in this country,” he said.
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