Customers in Cheshunt, Hertfordshire; Hatfield, Hertfordshire; Pentwyn, Cardiff; Southport, Merseyside; and Treforest, Rhondda Cynon Taf can now sign up to access Virgin Media's 100Mbps service.
Households receiving the superfast speed will be able to download an entire music album in around five seconds, or a TV show in around 30 seconds. A full high definition movie will take just seven minutes.
The rollout follows an initial service launch last month in Heckmondwike in West Yorkshire, the Hampshire town of Farnborough, Colchester in Essex and Barry in South Wales.
To promote the launch, Virgin Media unleashed a fleet of superfast taxi cabs in London, including a Porsche 997 Turbo Gen 1, a Ferrari 430 F1 Coupe and an Aston Martin DBS.
Virgin Media believes that the 100Mbps service ideally suits households with multiple persons online at any one time, using connected TVs, computers, games consoles or mobile smartphones.
According to the cable operator, the explosion in popularity of such devices has meant that data consumption on its network has increased by more than 215% in the past three years.
Jon James, executive director of broadband at Virgin Media, said: "From establishing the UK's first ever broadband service to the launch of 100Mbps just ten years later, Virgin Media has led the greatest developments in digital Britain.
"We've invested many billions of private money in order to build a growing network that already passes approximately 13 million homes across the UK. We're racing to get these ultrafast speeds across this entire area as fast as we can to meet demand."
As well as providing 100Mbps download speeds, the new service also delivers 10Mbps upload speeds, enabling users to share content such as live HD video. The package comes with a custom built combined modem and wireless 'N' router, which has the potential to deliver speeds of up to 400Mbps as new services roll out in the future.
Virgin Media claims that a "typical family" will be able to receive the 100Mbps service for £35 a month when bought with a phone line, or £45 per month without.