You can't add items to an already created MPMediaItemCollection. Instead you have to add them when you create the collection, using initWithItems:
or collectionWithItems:
.
You could "fake" adding an item by creating a new collection based off of the old one. Something like this:
NSMutableArray *items = [NSMutableArray arrayWithArray:myMediaItemCollection.items];
[items addObject:myNewMediaItem];
MPMediaItemCollection *myNewMediaItemCollection = [MPMediaItemCollection collectionWithItems:items];
(If your collections are going to live beyond the scope of the current method, you'll need to assign them to properties or call retain as appropriate.)