I've spoken to several different homeless folks, and almost all of them have said that hygiene items are some of the things that they need most. Here are a few ideas!
Snacks that are high in protein, as well as snacks that are easily portable, are ideal!
Necessary items of clothing that are highly-recommended!
Storage options for your care kits. This allows homeless folks to carry around both the kits that you provide as well as other items that they have accumulated.