The spa town topped the poll for the third year in a row in the Rightmove report, which asked 24,000 people how they feel about where they live.
Shrewsbury was ranked second, with Ipswich third and York and Chester completing the top five.
Inverness came highest in Scotland, in sixth, with seventh-placed Llandrindod Wells the top Welsh location.
Participants in the survey were asked to rate their area based on 12 factors, including neighbourliness, how safe they felt, recreational facilities, sense of community, living costs, contentment and how proud they felt about their home.
Richard Cooper, Conservative leader of Harrogate Borough Council, described the North Yorkshire town as a fantastic place to live.
"We are surrounded by some of the UK's most beautiful scenery, have fantastic shopping, a wide variety of restaurants and cafes and great entertainment and leisure opportunities, including some unique experiences such as the elegant Turkish Baths," he said.
"As a floral town, we are also extremely lucky to have a significant number of parks and gardens in the immediate vicinity, which are a joy to discover."
Hemel Hempstead ranked highest in the south-east of England, in eighth place, but London fared badly in the poll - with nine of the bottom 10 places in the capital.
Bottom of the list, in 130th place, was the east London borough of Barking and Dagenham.
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Darren Rodwell, the Labour leader of Barking and Dagenham Council, said: "I find this report quite amusing as we have just had tens of thousands of people coming to a series of events celebrating 50 years of our borough.
"Of course there are challenges in Barking and Dagenham, like there is anywhere else in the country in this age of austerity, but I know we have the drive and ambition to make this borough a better place to live for everyone."
Harrogate is the happiest place to live in Britain, according to a survey by a property website.