How to modify existing contact records to update their company information?

Are you updating the “Company ID” on the contact with “Company ID” of the company you want contact associated with?

You can also “Mass Update” contacts by exporting contacts and changing desired information and then import the updates, see:https://help.infusionsoft.com/userguides/contact-management/import-contacts/modify-existing-contact-records-with-a-spreadsheet