The move follows NTL president CEO Barclay Knapp's decision earlier this year to move his office to the UK from New York, where he was previously based along with a number of NTL investors.
It also comes ahead of the completion of NTL's refinancing deal that was agreed with shareholders and which will see £7.4bn wiped off the company's £12bn debt pile.
Carter said: "We have achieved an enormous amount over the last two years, delivering broadband leadership and positive operating cash flow. With Barclay now based in the UK and returning to full-time operations, and with NTL on track to emerge from US Chapter 11 in November I feel the time is right to move on."
Carter joined the company in September 2000 from WPP-owned advertising agency J Walter Thompson where he was chief executive. Since his appointment at NTL, Carter has overseen the integration of the former Cable & Wireless Communications into NTL and worked at reducing costs at the company.
Knapp said "Over the past two years, Stephen has achieved a great deal at NTL. We are now the clear leader in broadband with 40% market share and our earnings before tax, interest, depreciation and amortisation margin has increased from 11% in 2000 to 28% in our latest quarterly results. I am sad to see Stephen go and I wish him well."
The decision will fuel speculation that Carter is in the running for the vacant chief executive role at media group Emap, after weekend newspaper reports suggested he was among a shortlist of high-profile names being lined up for the job.
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