No, it won't hurt anything. but something changed... Do you know what?
What are your speakers and their rated FR?
I'm a big fan of seting the XO to 1 octave above the lower end of your FR... so if your speaker is rated at 40 Hz, I set my XO at 80. If its 60Hz, I set it at 120. (An octave above is a doubling of the frequency.)
But the most important part is to listen to it!
Try setting your surrounds up as mains for a little. Set the XO and listen to some music to see how it sounds. Adjust it up and down a few times. Is there a particular setting where the bass and treble sound cleaner?
I have a pair of speakers rated at 34Hz that left me struggling between 60 and 80. After a little listening, I heard an improvement in SQ in the way of punchier bass response and more midrange clarity. 80Hz won out!
Experiment and listen!