This site has TONS of resources for structured play, beginning literacy activities, and hand-eye coordination broken down by age from birth and through school years. Stoplight Beanbag Toss - I Can Teach My Child! I own bean bags already!
DIY Portable LEGO Kit with 24 Free Printable Activity Cards. A great idea for those times where you have to wait (Doctor's office, restaurant) or when you are traveling (great in the car or on a plane)! From Fun at Home with Kids