If you're talking about city living, it's Albany by a mile.
Hartford sucks as a city, mainly because it was horribly urban renewed - quite possibly the worst example of urban renewal in New England. Much of the historic building stock was knocked down in Downtown to make it into a vertical office park. The portions of Downtown to the west still have a ton of surface parking lots. There are a growing number of Downtown condos/apartments, but due to the limitations of the rest of the city, this doesn't matter that much.
Downtown is separated from the residential portions of Hartford by a ring of highways, along with a swathe of parking lots and institutional buildings. The residential neighborhoods which survived are mostly not particularly urban in character, with the exception of portions of Frog Hollow. They are almost all low-income, majority minority neighborhoods as well, with nearly the entire southern portion of Hartford overwhelmingly Latino, and the entire northern end overwhelmingly black. The West End is the only desirable portion of residential Hartford, and it is a long walk from Downtown, and basically suburban in nature. There are no gentrifying neighborhoods.
In contrast, while Albany was hit hard by urban renewal, a lot survived. Yes, Empire State Plaza took out much of the heart of Albany. But it still has a mostly intact, historic downtown. More importantly, it still has Center Square, a urban, walkable, and desirable neighborhood.
Hartford has nothing to compare to this. It's like a little bit of Manhattan was plopped down into Upstate NY. There are plenty of other examples of not gentrified urban neighborhoods as well, not only in Albany, but in nearby Rensselaer, Troy, etc. Not so much Schenectady though.