My DS1 will yell at DS2 and then smack him around the head or body. Not generally hard, but still - it's not on. I put him straight into time out and make no bones about being unhappy with his behaviour. Sometimes he gets a smack. To try and get through to him why it's not nice I say "he's your little brother - you have to look after him, he just wants to play with you, you have to share, it's not nice to hit etc etc etc". It's not constant here, but the minute DS2 takes another of DS1's toys, it happens again.
I can see you've tried time out, among other things. While it's not nice, it's obviously a stage most of them go through and I guess all you can do is be as consistent as you can with the "punishment" when your DD does it. Sorry I can't offer any other pearls of wisdom.
Usually if we have a toy delema, i ask DS to choose a toy that baby can play with, he thinks that is heaps of fun and will often give her his own toys or one of hers. He does get possesive though and has at the odd time tried to sit on her for fun!! I think the older ones are just learning what they can do with the new baby who is now suddenly moving and crawling and wanting to touch everything!!
Have you tried putting DS in a playpen by himself with some toys. That way he can stay in the play room with DD but she will have trouble getting to him to hurt him.
I agree with getting DD to choose some toys that are special to her and then creating a special place for her to put them, in a pretty decorated box, in her room etc. Then talk to her about the rest of the toys being for sharing.
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