It's just saying that whatever data-model object that NSObjectController is using does't have an appropriate key method for that value.
From looking at the Cocoa Bindings Reference documentation, the value binding should be set to a key in your NSObjectController that corresponds to a key-value-coding compliant key in its model.
Example:
NSObjectController mode is Class, Class Name is foo. Then you bind foo's key of comboSelection to the NSComboBox's value. What the exception is saying is that the Foo class doesn't have a method called comboSelection:
- (NSString*)comboSelection;
- (void)setComboSelection:(NSString*)inSelection;
In the case of using a NSMutableDictionary as the NSObjectController's class, it's much easier, since the dictionary can hold arbitrary keys.
If you're using CoreData (mode = Entity), then your CoreData entity must contain the appropriate property.