If you don't already have this setup, just review the 'Setup Steps' in the "Sync The Home Folder Between Macs Using Chrono Sync" Guide.
Many of the steps performed can be accomplished by using a standard file sharing connection and you technically don't need to install Chrono Agent.
Also, you can read Joe Kissell's article on how to Merge two i Tunes Libraries.
Of course, this all assumes that you don't already use i Cloud/i Tunes to keep your i Tunes Libraries in sync.
There is a structured set of steps that must be followed to use Chrono Sync for the Music folder which contains the i Tunes Library.
This guide covers the steps necessary to successfully sync the Music folder between two macs.
Never attempt to sync files outside of the home folder such as 'Applications', 'System', or 'Library' between two Macs.
Problems can arise if Applications, or System files are synced that can easily result in application failure or a corrupt OS.
You need to start with an empty Music folder so that the first sync will result in everything from the Master Library on the Chrono Sync Mac replacing all Music files and folders on the non-Chrono Sync Mac.
However, Chrono Agent offers better performance, security and reliability versus a standard file connection.
It also eliminates common problems, such as permission errors, that typically occur when using standard file sharing.
In syncing two Macs, the focus needs to be on the home folder and the data files stored therein.
Make sure you have the same version of i Tunes on both Macs in order to synchronize the Music folder which contains your i Tunes Library.
Chrono Sync cannot merge two dissimilar i Tunes libraries.