Oh boy... seems to work now. I was so focused on needing two loops to do the job that I couldn't realize that only one loop was all I needed:
for (int i = 0; i < 4; i++)
{
byteArray[i][0] = (int)((myValues[i] >> 24) & 0xFF) ;
byteArray[i][1] = (int)((myValues[i] >> 16) & 0xFF) ;
byteArray[i][2] = (int)((myValues[i] >> 8) & 0XFF);
byteArray[i][3] = (int)((myValues[i] & 0XFF));
}
Both, the index for my rows and the index for the values happen to be the same and the column index can be hardcoded. Maybe not the most elegant solution but that's fine for me right now.