Well educational stuff always goes over well with parents. When my wife and I were looking for a good sitter, we looked for teaching experience, espically with the appropriate age group. Phonics are very cool. We also looked to people with alternative to watching TV for 6 hours a day. Healthy kids are kids who are engaged by other people, not Blues Clues or Mr. Rodgers (relationships with TV characters are rather one sided, and our daughter is going to grow up in a society of other people that she needs to interact with). To those ends: phonics and other learning bases materials are a must. While that may not be appropriate for an 18 month old, the 4 year old is probably ready to start reading and writing (if she hasn't already, I mean the father is an English prof). Board games are also good for the 4 year old. As far as the 18 month old goes, classic reading materials like Goodnight Moon are excellent. Teaching the 18 month old the names of objects in his life will help him quite a bit. You might also want to have flash cards with pictures of things (a house, a bird, a plane) to assist in the verbal skills.
You might also bring elementary movement based games to the table. Hide and seek (not hide and go seek tag, mind you) is a very active and engaging sport for a 4 year old, and if the 4 year old hides in sight her little brother, all the better. Things like that tend to develope comrodary between siblings.
Just a few ideas, and I'm sure you'll do great!
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