I couldn't test this because i'm not on a Mac (sorry if I misspelled something), but:
NSDictionary *dic1 = [NSDictionary dictionaryWithObjectsAndKeys:@"GOD", @"WORD", [NSNumber numberWithInt:8], @"SCORE", nil];
NSDictionary *dic2 = [NSDictionary dictionaryWithObjectsAndKeys:@"DONG", @"WORD", [NSNumber numberWithInt:16], @"SCORE", nil];
NSDictionary *dic3 = [NSDictionary dictionaryWithObjectsAndKeys:@"DOG", @"WORD", [NSNumber numberWithInt:8], @"SCORE", nil];
NSDictionary *dic4 = [NSDictionary dictionaryWithObjectsAndKeys:@"XI", @"WORD", [NSNumber numberWithInt:21], @"SCORE", nil];
NSSortDescriptor *scoreSort = [NSSortDescriptor sortDescriptorWithKey:@"SCORE" ascending:NO];
NSSortDescriptor *wordSort = [NSSortDescriptor sortDescriptorWithKey:@"WORD" ascending:YES];
NSArray *sortedArrayOfDic = [[NSArray arrayWithObjects:dic1, dic2, dic3, dic4, nil] sortedArrayUsingDescriptors:[NSArray arrayWithObjects:scoreSort, wordSort, nil]];
NSLog(@"%@", [sortedArrayOfDict valueForKeyPath:@"WORD"]);
This would do the same but a bit reduced and avoiding an iteration.