STOP TRYING TO GET A JOB.
Companies don’t give jobs away anymore. Which means unemployed or underemployed people should stop trying to get them. Telling an organization that you’d like to work for them is all but useless, because paying someone just for being enthusiastic is impractical. Companies are paying for talent.
So stop trying to get a job, and start trying to give your talents. First off, it forces you to clearly and realistically define what you’re capable of. But most importantly, it shows an organization that you are more concerned about what you can do for them than what they can do for you.
Ironically, this makes you even more valuable.