You can not do anything to the existing RAID 10 or 0+1 if you like, array as that is the only configuration that works as a RAID 10

However, if you want to add another RAID array to your existing RAID Host Controller, then you should be able to do that.
Do you have a dual-channel RAID controller, say a nice Adaptec board ?!?
If so then add the larger 73~74GB capacity drives to that channel and create a new RAID array. My suggestion is to use a RAID 5 with a hot spare/fix as this will give you striping+mirroring+parity and supports the above mentioned hot spare option

Also note that a RAID 5 array requires a minimum of 3 HD's and of course an extra HD for any hot spares.