What are people looking for on your site? These terms are keywords in the vocabulary of your actual audience and should definitely be added to your keyword list. Do not forget to look at the keywords people filled in that didn’t get any results: this was stuff people were expecting but didn’t find. You can look into the results of your internal search in Google Analytics at Behavior → Site Search → Search Terms.
Long Tail Pro is a keyword research tool that helps you quickly find low competition keywords for your website. In particular, the tool is built for people doing SEO (search engine optimization) as opposed to people doing paid ads (Google Adwords PPC). I'm sure there are some advertisers that use the tool for paid ad keyword research, but the tool was built for SEO keyword research.