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Definitely go with natural syntax. Google can figure out what the page is about without having to sacrifice readability. In fact don't overdo it with the frequency - just having the phrases in the title tag and a couple of times on the page is plenty.

I agree with David in that variety is the key. I also think that Google is doing a much better job at determining local intent in queries. I would make sure to build links without the geographic modifier as well. In fact, I would think that too many links with geo-modifiers may be a spam signal if it isn't already. Additionally, be sure to include lots of "stop" words in your anchor text along with verbs, adjectives, etc. Things like "a painter in Texas" or  "recognized as a top painter" are phrases that real people would use to link to a real site rather than "painter Texas."

You definitely want to build links with the company or personal name and include the keywords next to it as Google can definitely discern the proximity of the keyword and score it accordingly.

For example: Joe Bob is a Texas-based painter...

Hope that helps!

Stop hoarding the link juice and link out to related sites! Not so much a secret but something that is too often overlooked.