Some of my other favorites (as far as donating items and money):
Boston Children's Hospital
St. Jude's Childrens
local pet shelters (no-kill shelters)
American Cancer Society
I pretty much like to give to children causes and animals - I am a sucker for any kids asking for money outside of stores, I give to pretty much all the local kids looking to support their sports programs, girl scouts and cub scouts. I always wondered who those mean old adults are that can walk by those kids without dropping in a dime.
As far as time - similar sort of things - currently I am a pen pal with an elementary school boy, I've read to kids during my lunch time, I've held a clean up day at the local zoo, helped at elderly housing to spruce things up and hold parties, held Christmas parties with Santa at local city day cares, diaper drives, raised money/care packages for our service men overseas. I just wish I had more time to offer - the unfortunate thing is I don't have the time to do too many consistent things - more like one time stuff.