While most are not legally binding, there may still be consequences for not complying with the agreed upon portions of the letter. A Letter of Intent is often seen like purchase or crowd-sourced orders, so they are often used to help secure funding or prove the value of the business. If the other party drops out or doesn't honor "in good faith" the letter, actual financial damage may be incurred to the company. In court, most often the judge will make decisions based on what implied intent is expressed in the letter. Sometimes there can be recourse if the parties do not follow through towards an actual legal agreement.
Here's where the difference comes in between a cover letter and a letter of intent. With a cover letter, you likely already have a solid idea of what the job opportunity is, and how to position yourself for it. With a letter of intent, you have to make a slightly trickier balance—positioning yourself as qualified for a job that may not be clear yet. To do that, align your self talk around the company or the industry, making sure to highlight your skills and achievements that would make you a good fit for the company. You can also be specific about your level and experience. For example, you should make it clear that you're looking for a manager-level position if you don't want to be considered for more junior or entry-level roles.