I lived in Santa Fe for 15 years. It's a great pace to walk and to live for that matter, but you really could not live there without a car. It really is very small and isolated (60 miles from Albuquerque which isn't much of a city, and 400 from Denver). At 121,593 sq mi, New Mexico is the fifth biggest state in the US. It only has 2 million inhabitants making wilderness and natural beauty among the strongest draws in the Santa Fe area and State in general.
Of the large cities, your list is probably pretty accurate IMO.
Your description of Santa Fe reminds me of Portland, Maine where I've spent 4 years. Nice, small, quaint, surrounded by natural beauty (albeit, a vastly different type), and certainly isolated (around 100 mi from Boston). A car is absolutely necessary here unless you don't plan on leaving your block.
On topic- I agree with most of j6p's assessment of what makes a city a great place. While I won't pretend to have ever been part of "gritty" Boston, I've experienced what gritty and tough neighborhoods (slums) have to offer elsewhere and in my experience, Boston has a good balance of refinery and grit, though it does tend to lean to the former.
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