I occasionally cook meals for our local homeless shelter through our church. The first time, DH and I also helped served the meal. It was heartbreaking to see the many faces, a few were people I recognized.
I made a nice dessert to go along with the main dish, and they weren't very interested in that, because most were so hungry they wanted to fill up on the healthy meat and veggies.
It's located near the university and they usually get about 40 per night, but I know they must be just barely touching the surface of all the homeless and/or hungry folks in our area.
Some good things to donate to a shelter are diapers and new pillows. I prefer to cook a meal and try to make something special for them.