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.
In a nutshell, Long Tail Pro helps you quickly find keywords in bulk based on a seed keyword that you input. In addition to returning hundreds of related keywords, the tool also shows search volume (monthly search volume), advertiser bid, number of words, rank value, and my favorite Keyword Competitiveness (helps you judge the competition and keyword difficulty).